IT’S SATURDAY MORNING in Rio de Janeiro. The street sweepers in Lapa, the beating heart of Brazil’s second largest city and home to its most famous club, Rio Scenarium, are still clearing up the remnants of last night’s boisterous revelry. Disco throbs have turned into a gentle buzz as stalls line the streets for a weekly craft fair.

Like most people, I came to Rio in search of some samba and sun but my quest takes an expected twist after talking to one of the staff at Hotel Fasano, where I’m staying. She tells me that the piece we’re sitting on–a luxurious gray velvet sofa–belongs to Rogerio Fasano, the hotel group’s founder, who has been accumulating local treasures for years. The lobby is packed full of his furniture: a table hewn out of half a trunk of jacaranda wood, stylish sofas and sleek chairs with polished wooden arms.

With my own remodel under way at home in London, my appetite is whetted for some midcentury finds. And with the World Cup just around the corner, it feels like a particularly good time to be lapping up all things Brazilian–and a great excuse to spend a few days perusing the back streets of Rio.

The 1950s and ’60s were golden years for Brazilian design, with local Modernist heroes Sergio Rodrigues, Joaquim Tenreiro and Oscar Niemeyer capturing the zeitgeist–and winning fans across the globe–with their clean lines, lightness of form and unique woods. But their production was on a much smaller scale than the works of their European and U.S. counterparts, making them hard to come by. Good thing I’m in a the mood for a challenge.

After a bit of research, I find out that apart from auctions–which can be tricky to negotiate if you aren’t based here–Rua do Lavradio, the lifeline of Lapa, is also the main drag for shops specializing in midcentury furniture.

My first stop is Mercado Moderno ( 130 Rua do Lavradio; ), which comes highly recommended by a number of interior designer friends. Owner Marcelo Vasconcellos walks me around his shop, jam-packed with beautiful pieces.

A three-legged chair catches my eye. A Tenreiro ( $250,000/EUR180,000), it has a gently curved back that tapers elegantly and three different types of wood arranged in stripes, giving it a beautifully graphic focus. Then there’s a boxy, high-backed Poltrona Paulistana chair and footstool by Jorge Zalszupin from 1960 that reminds me of the Eames chair ( 30,000 Brazilian real/$13,450/EUR9,600). Nearby, an Oscar Niemeyer wicker chaise longue from 1970 balances on a curved piece of wood ( 60,000 real).

Mr. Vasconcellos says interest in such pieces has been steadily growing. “There is a strong movement in Brazil to increase the value of this market,” says Mr. Vasconcellos, whose passion for midcentury furniture from Brazil has led to a book on the subject, “Móvel Brasileiro Moderno (Brazilian Modern Furniture),” as well as an exhibition he co-curated last year at the National Historical Museum. “Another factor which strengthens the allure of vintage furniture is the attention which contemporary furniture is getting, with names such as Irmãos Campana, Zanini de Zanine and Rodrigo Almeida.”

Next, I head to Ateliê Belmonte ( 34 Rua do Lavradio, ), a two-story shop where brightly colored Space Age chairs mingle with more down-to-earth wooden pieces. When I enter, two men are taking the pick of the shop for their Paris apartment, and it’s easy to see why. Even the ashtrays seem effortlessly chic.

“The ’60s was an age when the modern design in Brazil was very creative, ” says owner Luciano Cavalcanti de Albuquerque, who also has a design studio and architecture practice above the store. “Today this furniture is particularly up-to-date and fashionable.”

He’s right there. I immediately covet a 1960s curved orange armchair ( 1,900 real) made by Gelli, a well-known Petrópolis factory. And there’s a Luxor chair with sleek wooden arms ( 2,900 real) and a jacaranda and straw mesh chair ( 1,400 real) that would look right at home in my London living room. But many of Mr. Cavalcanti de Albuquerque’s best finds never even make it onto the showroom floor. He keeps a collection of rare furniture that goes directly to clients. For a look at these pieces, ask in advance.

Further down the road at No. 128 is Mobix ( +55 21 2224 0244), where classic 1960s pieces like Sergio Rodrigues’s Moleca chair ( 13,000 real) sit alongside recently made Modernist-style furniture. The shop is one of the most well-edited collections on the street, with uniformly covetable pieces, and I find it hard to resist a pair of heavy rosewood chairs ( price upon request).

Nearby, across from Rio Scenarium, at number 11, Costanza Assereto, a Turin native, has furnished her restaurant, Casa Momus ( ), with midcentury finds from the neighborhood. Among her prize possessions is a Sergio Rodrigues table. “The combination of proportions, materials–chrome steel and jacaranda, when it was still legal to use it–and refined simplicity just mesmerized me,” she says.

Despite a fun day of shopping, I am leaving Rio empty-handed–for now. But I plan on staying in touch with Mr. Vasconcellos, and seeing if I can’t get that Niemeyer chaise longue shipped to London. Perhaps alongside the Rodrigues jacaranda chairs, too. Because everyone needs a little Copacabana at home.