Jabarkan 1959–1971: Masa Kejayaan dari Ray Charles

Charles reached the pinnacle of his success at Atlantic with the release of "What'd I Say", which combined gospel, jazz, blues and Latin music. Charles said he wrote it spontaneously while he was performing in clubs with his band. Despite some radio stations banning the song because of its sexually suggestive lyrics, the song became his first top ten pop record.

Later in 1959, he released his first country song (a cover of Hank Snow's "I'm Movin' On") and recorded three more albums for the label: a jazz record (The Genius After Hours, 1961); a blues record (The Genius Sings the Blues, 1961); and a big band record (The Genius of Ray Charles, 1959) which was his first Top 40 album, peaking at No. 17.

His contract with Atlantic expired in 1959, and several big labels offered him record deals; choosing not to renegotiate his contract with Atlantic, he signed with ABC-Paramount in November 1959. He obtained a more liberal contract than other artists had at the time, with ABC offering him a $50,000 (US$ in  dollars) annual advance, higher royalties than before and eventual ownership of his master tapes—a very valuable and lucrative deal at the time. During his Atlantic years, Charles had been heralded for his inventive compositions, but by the time of the release of the largely instrumental jazz album Genius + Soul = Jazz (1960) for ABC's subsidiary label Impulse!, he had given up on writing to follow his eclectic impulses as an interpreter.

With "Georgia on My Mind", his first hit single for ABC-Paramount in 1960, Charles received national acclaim and four Grammy Awards, including two for "Georgia on My Mind" (Best Vocal Performance Single Record or Track, Male, and Best Performance by a Pop Single Artist). Written by Stuart Gorrell and Hoagy Carmichael, the song was Charles's first work with Sid Feller, who produced, arranged and conducted the recording.

Charles earned another Grammy for the follow-up "Hit the Road Jack", written by R&B singer Percy Mayfield.

By late 1961, Charles had expanded his small road ensemble to a big band, partly as a response to increasing royalties and touring fees, becoming one of the few black artists to cross over into mainstream pop with such a level of creative control. This success, however, came to a momentary halt during a concert tour in November 1961, when a police search of Charles's hotel room in Indianapolis, Indiana, led to the discovery of heroin in the medicine cabinet. The case was eventually dropped, as the search lacked a proper warrant by the police, and Charles soon returned to music.

In the early 1960s, on the way from Louisiana to Oklahoma City, Charles faced a near-death experience when the pilot of his plane lost visibility, as snow and his failure to use the defroster caused the windshield of the plane to become completely covered in ice. The pilot made a few circles in the air before he was finally able to see through a small part of the windshield and land the plane. Charles placed a spiritual interpretation on the event, claiming that "something or someone which instruments cannot detect" was responsible for creating the small opening in the ice on the windshield which enabled the pilot to land the plane safely.

The 1962 album Modern Sounds in Country and Western Music and its sequel, Modern Sounds in Country and Western Music, Vol. 2, helped to bring country music into the musical mainstream. Charles's version of the Don Gibson song "I Can't Stop Loving You" topped the Pop chart for five weeks, stayed at No. 1 on the R&B chart for ten weeks, and gave him his only number-one record in the UK. In 1962, he founded his record label, Tangerine, which ABC-Paramount promoted and distributed.  He had major pop hits in 1963 with "Busted" (US No. 4) and Take These Chains from My Heart (US No. 8). In 1964 Margie Hendricks was kicked out of The Raelettes after a big argument.

In 1964, Charles's career was halted once more after he was arrested for a third time for possession of heroin. He agreed to go to rehab to avoid jail time and eventually kicked his habit at a clinic in Los Angeles. After spending a year on parole, Charles reappeared in the charts in 1966 with a series of hits composed with Ashford & Simpson and Jo Armstead, including the dance number "I Don't Need No Doctor" and "Let's Go Get Stoned", which became his first number-one R&B hit in several years. His cover version of "Crying Time", originally recorded by country singer Buck Owens, reached No. 6 on the pop chart and helped Charles win a Grammy Award the following March. In 1967, he had a top-twenty hit with another ballad, "Here We Go Again".