In 1964 the album Guitar From Ipanema won the grammy for Best Instrumental Jazz Performance. Almeida’s recording career enjoyed auspicious early success with the 1953 recordings now called Brazilliance No. 1 and No. 2 with fellow Kenton alumnus Bud Shank, bassist Harry Babasin, and drummer Roy Harte on the World Pacific label (originally entitled “The Laurindo Almeida Quartet featuring Bud Shank”). Widely regarded as "landmark" recordings, Almeida and Shank’s combination of Brazilian and jazz rhythms (which Almeida labeled "samba-jazz") presaged the fusion of Latin and jazz, which is quite different in bossa nova, although jazz critic Leonard Feather credited Almeida and Shank as the creators of bossa nova sound
Other observers note that the beat, harmonic stamp, and economy of expression were different than the bossa nova, giving Almeida and Shank's recording "...a different mood and sound...certainly valuable in its own right."
Almeida’s classical solo recording career on Capitol Records began in 1954 with The Guitar Music of Spain. Almeida made a series of highly successful classical recordings produced by Robert E. Myers. Among Almeida’s notable classical recordings is an album widely considered to be the first classical crossover album, the 1958 Grammy winner Duets with Spanish Guitar with mezzo soprano Salli Terri and flutist Martin Ruderman. In this recording, Almeida arranges standard classical and folk repertoire through the prism of several Latin musical forms, including the modenha, charo, maracatu and boi bumba. The result, according to Hi-Fi and Music Review was "...a prize winner in my collection. Laurindo Almeida’s guitar playing captures the keen poignancy and rhythmic élan of Brazilian music with superb assurance and taste...". The recording was nominated for two Grammy Awards and won for Best Classical Engineering for Sherwood Hall III at the first Grammy Awards ceremony.
Classical and jazz guitarist and composer Laurindo Almeida was a key player in fusing spicy Brazilian music with cool jazz to create the bossa nova music that was so popular during the mid '60s through the early '70s. At the height of his popularity, Almeida himself scored a few major feature films and assisted on the scores of others.