This morning you'll head to the airport for your hour-long flight to Sucre where you'll transfer from the airport to the heart of this UNESCO-protected colonial city. At around 9,000 feet above sea level, Sucre's whitewashed buildings and narrow cobblestoned streets, make it the perfect place to rest and acclimate before heading higher up into the heart of the Bolivian highlands. Sucre was once the home of the Spanish aristocrats who were made rich by the silver mines of Potosí but came to this temperate valley to escape the harsh climate near the mines. You can spend the afternoon strolling the bustling streets of this now-college town and pausing in quiet plazas under the stone walls of centuries-old cathedrals and mansions.

After a day of resting and getting used to the rarified air of Sucre, you'll now have the spring in your step needed to ascend to the stone arcades of the Recoleta. There you can sip a coffee as you take in the sweeping view of the city and the jagged peaks of the Cordillera de los Frailes. Or you can venture straight into the heart of the city's activity by going to the central market. Don't pass up an opportunity to sample a chirimoya, a fruit that looks like a gigantic green strawberry and has a sweet, custard-like texture.

Today you'll trade the white walls of Sucre for the towering red-rock wall of the Maragua Crater and its bizarre geology and rich culture. The greens of the plots of crops, plowed by hand with oxen, make the red sandstone strata glow even more vividly, but no scarlet hue is brighter than that of the Jalq'a tapestries hand-woven in the homes of the crater's villages. As you pass, Quechua villagers may lay down their hoe or shepherd's crook and invite you in their adobe hut to show you how they use their loom and shuttlecock to bring the complex designs into being. But as ancient as the current way the crater's inhabitants live today may seem, the crater has born witness to yet older happenings. It was here that over two centuries ago indigenous revolutionary leader Tupac Katari was executed. And to go back even further, keep your eyes peeled for fossils in the petrified Jurassic mud beds exposed by the rains and winds of the crater.

The three-hour drive in a private car from Sucre to Potosí takes you deep into the gorge of the mighty Pilcomayo River and up onto the high plateau of Potosí—13,000 feet above sea level. In its heyday several centuries ago, the city of Potosí rivaled the largest capitals of the world in terms of population and splendor, a past still visible in its ornate stonework. After lunch, find your way to the Casa de Moneda museum for a vivid portrayal of this past. Among many other artifacts and artwork that tell the city's story, the museum features the donkey-powered mint where the Spanish made the silver coins, the world's first, real global currency.

Above Potosí's stone mansions and cathedrals and adobe and cinder-block walls and tin roofs of its outskirts, rises the Cerro Rico mountain. Cerro Rico holds veins of silver so rich that they continue to be mined 500 years after their discovery. Learn how little the mining methods have changed since then on a tour of the mine. After loading up on coca leaves and other gifts for the miners in the market, you'll be outfitted with a hard hat, light, and coveralls. You'll then venture down the twisting, anthill passageways to where crews hack at the stone walls with their pickaxes. If you are feeling inspired, leave a gift for the Tío statue, the god of the underworld and mines to which the miners pray for safety and fortune. In the afternoon, you'll make the scenic four-hour transfer to Tupiza, the jumping-off point for exciting excursions into the wild and remote lands of Sur Lípez.

The lanscapes around Tupiza look just like the Wild West with its impressive canyons and red rocks. So get the best of it riding a horse in the amazing scenary of Quebrada de Palmira, the coloured vertical mountains to La Puerta del Diablo and Valle de los Machos. You have the rest of the day to relax in Tupiza.

After leaving the red-rock canyons of Tupiza, the road winds up through spires and over a rock causeway with sheer drops on either side. The broken edges of the high plateau of the Andes rise to vast basins bordered by hulking volcanoes. On the barren slopes of one volcano the wind hisses through the abandoned stone city of San Antonio de Nuevo Mundo, once a booming silver mining center in the 1600s. The road continues across rivers and llama-filled plains to Quetena, a village of herders set among slot canyons with startling green Andean peat-bogs. Above it is the Uturunku volcano, the highest in the area, and, according to an international study, a supervolcano sitting atop a pool of magma the size of Lake Superior.

Rise early and head to the Sol de Mañana geyser field, where you can jump through plumes of warm steam hissing up through subterranean cracks and wander alongside scalding mud pots. The streams with no geothermal source may be iced over and sparkling like jewels strung out across a desert, but you won't have to suffer from the cold. The waters of the Polques Hot Springs will be steaming and welcoming. After a relaxing soak, the journey continues south to the Dalí Desert, with strange formations and lines that remind the painter's surrealism. Beyond the desert are the emerald waters of Laguna Verde, at the edge of the Chilean border. When it's time, you'll make your way to your hotel near Laguna Colorada, the crown jewel of the high lakes in the region where its salty blood-red waters teem with flamingos and fill the silence of these harsh lands with their cacophonous din.

At dawn, you'll skirt the edges of Laguna Colorada heading north to the Árbol de Piedra (the Tree of Stone). Looking more like petrified trees, the twisted rock formations in the area shelter mounds of green moss further adding to the alien landscape. The route passes by a string of high-altitude lakes—Cañapa, Hedionda, Ch-arkota, Honda, and Ramaditas—each with their distinct coloration and waterfowl, including three species of flamingo. As the route descends slightly and leaves the harshest high-elevation terrain behind, keep your eyes peeled for the vicuña, a sleek, wild cousin of the alpaca and llama, or the ñandu, an Andean ostrich. The backdrop for these animals becomes more and more magnificent as you near the Ollagüe volcano, a massif on the Chilean border belching great clouds of sulfurous smoke. After crossing the salt flats of Chiguana, you'll arrive at the village of San Juan for the night.

From San Juan, you'll venture across Salar de Uyuni (salt flats), an immense white expanse the size of Connecticut and the flattest place on planet earth. You can use the endless horizon to take pictures that play with perspective, and a thin layer of rainwater turns the flats into a perfect mirror, suspending you in an ethereal world of sky and clouds. From there, you'll stop at the cactus-studded Isla Incahuasi (Incahuasi Island). Here you can climb through the spines and twisted boulders to the island's peak to appreciate the vastness of the Salar and walk the desiccated shoreline to examine the intricate geometry of the cracks in the salt to get a sense of the vast solitude of this desert wasteland. The journey then continues to Uyuni, where you will take an eight-hour sleeper bus to La Paz.

You'll have today to catch your breath (or have it taken away) as you plunge into the colorful bustle of La Paz. With houses spilling down the canyon walls at 12,000 feet above sea level below the glaciated hulk of Illimani Mountain, La Paz is a jumble of tradition and modernity. Cholitas (women in typical dress dating back to colonial times) float serenely over the chaos in the world’s most modern urban gondola system, Mi Teleférico. Wander the maze of steep streets and stairways, visit the number of museums and markets, like Witches Market, and be sure to check out the historic downtown and lively nightlife.

After driving along the shores of Lake Titicaca under the glaciers of the Cordillera Real, and crossing the Straights of Taquina on rustic barges, you'll arrive at Copacabana. The main port town on the Bolivian side of the lake, Copacabana has an ornate basilica with a black Virgin Mary waiting for you to discover. From Copacabana, you'll take a boat to Isla del Sol (Island of the Sun) and ascend the 500 steps of the famous Escalera del Inca staircase to viewpoints overlooking the beautiful azure waters below. A local guide will take you along the crest of the island above the terraced slopes, still farmed by the Aymara people, recounting legends and myths. As the light fades, you can enjoy the sunset over the highest navigable lake in the world.

After visiting the Inca temple of La Chinkana, the most important Inca ruin on the south side of Isla del Sol, you'll take a boat to the lesser-traveled Isla de la Luna (Island of the Moon), the female counterpart of the former. Here you can share a traditional apthapi "potluck" meal with the Aymara community, and see the landscape and archaeology of the island. Consider participating in the ancient reed-net fishing methods of the lake-dwellers before settling in for the night.

This morning you'll board a private boat and ride to the village of Yampupata on the mainland. From here you'll trek along the ancient stones of a pre-Colombian path. Three hours of hiking take you through Sampaya and Jinchaca, untouched by tourism, whose village residents will be hoeing their fields of purple-flowered tarwi beans or tending to their herds of llamas between the bright blue expanse of the altiplano sky and the sparkling waters of the lake. A vehicle will take you from the hike's end back to Copacabana, where you will board the return bus to La Paz.