Crosby briefly studied drama at Santa Barbara City College before dropping out to pursue a career in music. He performed with singer Terry Callier in Chicago and Greenwich Village, but the duo failed to obtain a recording contract. He also performed with Les Baxter's Balladeers in 1963. With the help of producer Jim Dickson, Crosby recorded his first solo session also in 1963, with a cover of a song by Ray Charles. Miriam Makeba was on tour and in Chicago at the time with her band, which included Jim McGuinn, a multi-instrumentalist who later dropped his first name and began to go by his middle name, Roger McGuinn. Callier introduced Crosby to McGuinn  and Gene Clark, who were then performing by the name the Jet Set. Crosby joined them, and they were augmented by drummer Michael Clarke, at which point Crosby attempted, unsuccessfully, to play bass. Late in 1964, Chris Hillman joined the band as bassist, and Crosby relieved Gene Clark of rhythm guitar duties. Through connections that Jim Dickson (The Byrds' manager) had with Bob Dylan's music publisher, the band obtained a demo acetate disc of Dylan's \"Mr. Tambourine Man\" and recorded a version of the song, featuring McGuinn's twelve-string guitar as well as McGuinn, Crosby, and Clark's vocal harmonies. The song turned into a massive hit, reaching No. 1 in the charts in the United States and the United Kingdom during 1965. While McGuinn originated the Byrds' trademark 12-string guitar sound, Crosby was responsible for the soaring harmonies and often unusual phrasing of their songs, but while he did not sing lead vocals on either of the first two albums, he sang lead on the bridge in their second single \"All I Really Want to Do\".
Friction between Crosby and the other Byrds came to a head in mid-1967. Tensions were high after the Monterey International Pop Festival in June when Crosby's onstage political diatribes and support of various John F. Kennedy assassination conspiracy theories between songs outraged McGuinn. He further annoyed his bandmates when, at the invitation of Stephen Stills, he sat in with Buffalo Springfield's set the following night, after Young had quit the band and was replaced by guitarist Doug Hastings. The internal conflict boiled over during the initial recording sessions for The Notorious Byrd Brothers (1968) that summer, where differences over song selections led to intra-band arguments. In particular, Crosby was adamant that the band should record only original material despite the recent commercial failure of \"Lady Friend\", a Crosby-penned single that stalled at No. 82 on the American charts following its release. McGuinn and Hillman dismissed Crosby in October after he refused to countenance the recording of a cover of Goffin and King's \"Goin' Back\". While Crosby contributed to three compositions and five recordings on the final album, his controversial ménage à trois ode \"Triad\" was omitted. Jefferson Airplane released a Grace Slick-sung cover on Crown of Creation (1968), and three years later, Crosby released a solo acoustic version on Crosby, Stills, Nash & Young's double live album 4 Way Street (1971). The Byrds' version appeared decades later on the 1987 Never Before release and later on the 1997 re-release of The Notorious Byrd Brothers.
In 1969, Neil Young joined the group, and with him, they recorded the album Déjà Vu, which peaked at No. 1 on the Billboard 200 and the ARIA Charts. On September 30, 1969, Crosby's longtime girlfriend Christine Hinton was killed in a car accident only days after Hinton, Crosby, and Debbie Donovan moved from Los Angeles to the San Francisco Bay Area. Crosby was devastated, and he began abusing drugs more severely than he had before. Nevertheless, he still managed to contribute \"Almost Cut My Hair\" and the album's title track. After the release of the double live album 4 Way Street, the group went on a four-year hiatus to focus on their respective solo careers.
CSNY did not perform together again as a foursome until Live Aid in Philadelphia in 1985, and then performed only sporadically in the 1980s and 1990s (mainly at the annual Bridge School Benefit organized by Young's wife Pegi). Without Young, however, Crosby, Stills & Nash performed much more consistently after its reformation in 1977. The trio toured in support of their 1977 and 1982 albums CSN and Daylight Again and then, starting in the late 1980s, toured regularly year after year. The group continued to perform live, and since 1982 released four albums of new material: American Dream (1988, with Young), Live It Up (1990), After the Storm (1994), and Looking Forward (1999, with Young). In addition, Crosby & Nash released the self-titled album Crosby & Nash in 2004.
As a duo, Crosby & Nash (C&N) released four studio albums and two live albums, including Another Stoney Evening, which features the duo in a 1971 acoustic performance with no supporting band. Crosby songs recorded by C&N in the 1970s include \"Whole Cloth\", \"Where Will I Be\", \"Page 43\", \"Games\", \"The Wall Song\", \"Carry Me\", \"Bittersweet\", \"Naked in the Rain\" (co-written with Nash), \"Low Down Payment\", \"Homeward Through the Haze\", \"Time After Time\", \"Dancer\", \"Taken at All\" (also co-written with Nash), and \"Foolish Man\". During the mid-1970s, Crosby and Nash enjoyed careers as session musicians, contributing harmonies and background vocals to albums by Joni Mitchell, Jackson Browne (whom Crosby had initially championed as an emerging songwriter), Dave Mason, Rick Roberts, James Taylor (most notably \"Lighthouse\" and \"Mexico\"), Art Garfunkel, Carole King, Elton John, J.D. Souther, and Gary Wright.
In 2006, Crosby and Nash worked with David Gilmour as backing vocalists on the latter's third solo album, On an Island. The album was released in March 2006 and reached No. 1 on the UK charts. They also performed live with Gilmour in his concert at the Royal Albert Hall in London in May 2006 and toured together in the United States, as can be seen on Gilmour's 2007 DVD Remember That Night. They also sang backup on the title track of John Mayer's 2012 album Born and Raised.
In July 2021, Crosby released what would become his final studio album, For Free. This was followed by the release of the 50th-anniversary expanded version of If I Could Only Remember My Name on October 15. It contains remastered songs as well as demos from the original recording sessions. During promotion for the rerelease, Crosby said that his second collaborative album with League, Stevens, and Willis was in the works. The result, Crosby's final release, was a live album recorded during the band's tour, Live at the Capitol Theatre, released October 4, 2022.
In 1996, Crosby formed CPR or Crosby, Pevar & Raymond with session guitarist Jeff Pevar, and pianist James Raymond, Crosby's son. The group released two studio albums and two live albums before disbanding in 2004.
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