OUR AHA moment came near the beginning of the trip, somewhere around 11,300 feet, in Argentina’s far north, along the narrow and steadily rising Route 33. My wife, Paula, and I had just reached the Cuesta del Obispo, or “Bishop’s Slope,” a mountain overlook with a closet-size stone chapel and a metal shack that served llama sausages and mounds of semihard goat cheese. As we chewed the gristly meat looking out at the mountainous vastness, we had our realization: We’d come for the wine, but we’d been so intoxicated by the scenery that we’d forgotten to pick up a bottle to drink.

Paula and I had been driving south for the last three hours from the provincial capital of Salta, most of it on twisting roads. Our mode of conveyance was an underpowered, dented, manual silver sedan that the rental agent must have reserved for Americans with dubious adroitness at driving a stick.

Three-quarters of Argentina’s increasingly acclaimed wine is produced in Mendoza, about 800 miles south of Salta, where Paula’s family had once been winemakers (she was produced there, as well). But we wanted to explore Argentina’s winemaking at its roots, which can be traced to the arrival of the Spanish conquistadors and Jesuits in Salta in 1534. Today, some 6 million gallons are bottled annually in Salta’s Calchaquí and Cafayate Valleys, making the province the country’s fourth-largest wine-producer, despite the challenges of growing grapes at high elevation (5,400 feet versus just 2,000 in Mendoza) and in such an arid and remote location.

It is also flat-out stunning. Not long after we’d left Salta, we were driving through green, cultivated fields filled with white butterflies pouring off them. This scenery soon yielded to neck-high pampas grass, then, just as suddenly, rock formations that appeared as if they’d just erupted from the earth, striated in red and yellow. “It is like being in a slideshow,” Paula said. “Each time you blink, the landscape’s different.”

The village of Molinos features Spanish colonial buildings with elegant white facades.

Heading farther west, skirting the northern edge of Los Cardones National Park, a 248-square-mile desert dotted with cardon cactuses that look like fingers reaching toward the sky, we entered an arid landscape of earthen spires and pyramid shapes. In the village of Seclantás, the colors of the llama-wool ponchos sold outside adobe workshops mirrored the green, ocher, violet and blue of the desert formations. After driving for six hours, we stopped for the night at an 18th-century hacienda in the village of Molinos, where the streets smelled of wild sage and the Spanish colonial buildings had elegant white facades.

Before dinner, we started with Torrontés and Malbec wines in the hacienda’s courtyard, before moving inside for sweet Andean corn tamales, empanadas, and a Salteño stew of lima beans, squash and sausage, followed by candied cuaresmillo peaches and figs in syrup. Sated beyond imagination, we slept like stones.

The following morning we headed to the vineyards, braving rutted gravel roads, often carved into cliffs. Our first stop was Colomé, site of the country’s oldest winery, which blends grapes from vineyards at four separate elevations. By now, we’d noticed that Salta’s producers don’t just list their alcohol content on their labels—they list their elevations, too. (Bodega Tacuil, just 9 miles away, is the area’s highest winemaking facility at 8,422 feet.) Before leaving, we toured Colomé’s private James Turrell Museum, which consists of nine luminescent, colored rooms.

Llama carpaccio at Bodega El Esteco Photo: Javier Pierini for The Wall Street Journal

Our favorite part of the day was the drive to Cafayate, through the Quebrada de las Flechas, or “Ravine of Arrows,” a narrow pass of rock formations towering up to 70 feet along Route 40. It was as if the desert had transformed into a jagged earthen sea, with waves frozen as they were breaking. Around sunset, we pulled into the Patios de Cafayate hotel beside the Bodega El Esteco winery (elevation 5,577 feet), whose Don David Reserve Malbec went down well with a dinner of llama carpaccio and glazed goat ravioli.

The following day we headed back toward Salta, through the Quebrada de Cafayate, another sandstone canyon whose rock formations have evocative names such as “the Devil’s Throat.” We stopped for the night in Salta but were now in a full-fledged romance with the open road. We continued the next morning 97 miles north to Purmamarca, in Jujuy Province, where the mineral pigments in the Hill of Seven Colors looked like scoops of ice cream—pistachio, mint, coffee, vanilla and cherry melting on top of each other.

Quebrada de Cafayate is a sandstone canyon whose rock formations have evocative names such as ‘the Devil’s Throat.’

Argentina’s high-altitude wines are aromatic and floral, with higher sugar and alcohol content and a greater concentration of tannins than those made at lower elevations. Many are excellent; some are world-class. But they weren’t the point. Or at least not the most important one. The jagged, soaring desert and mountain scenery that separated the vineyards turned out to be even more delicious than the wine. We were happy to sample just a few vintages at any one stop so we could get back into the car and keep going.

The Lowdown // Exploring Salta’s High-Altitude Wine Route

Getting There: Many carriers fly from the U.S. to Buenos Aires, including LAN and Aerolíneas Argentinas, both of which connect to Salta’s Martín Miguel de Güemes International Airport. Most major international car rental agencies have offices in the Salta airport but only offer cars with manual transmission.

Jason Lee

Staying There: In Salta, Legado Mitico is an elegant choice, and only a short walk to the central Plaza 9 de Julio (from $200, legadomitico.com). In Molinos, the 18th-century Hacienda de Molinos has modern bathrooms and a pool (from about $87 a night; haciendademolinos.com.ar). In Cafayate, the Spanish colonial Patios de Cafayate has sprawling rooms, llamas and a modern spa (from about $170 a night; patiosdecafayate.com). In Purmamarca, Hotel Manantial del Silencio has comfortable rooms, an excellent restaurant and an extensive wine list (from about $134 a night; hotelmanantialdelsilencio.com).

Drinking There: The region’s hallmark white is Torrontés; the principal reds are Malbec, Cabernet Sauvignon and Tannat. Top recent vintages are 2007, 2010 and 2011, while 2014 may be just as good. Outside Molinos, visit Colomé, the country’s oldest winery (built in 1831) and its James Turrell Museum (bodegacolome.com); Bodega Tacuil (tacuil.com.ar) is closed to visitors but worth the drive. In Cafayate, visit Piattelli Vineyards (piattellivineyards.com), Finca Quara (fincaquara.com), Bodega Domingo Molina (domingomolina.com.ar) and Bodega El Esteco (elesteco.com).