In 1941, the family moved to Wilmington, California but her parents divorced and times were hard. Carol worked hard whenever she could to help her mother and when she was 13, her mother scraped together $10 to buy a lap steel guitar and a couple of lessons. She was a natural and progressed to Spanish-style guitar at 14. Her teacher saw her potential and asked her to help him teach others. Carol started performing bebop jazz guitar with several bands around Long Island and there she met Al Kaye. In time the two were married and she took her husband's name to become Carol Kaye, and both played and toured the US with the Henry Busse Orchestra in the mid-50s. In 1957, Carol Kaye was recruited by Robert A. "Bumps" Blackwell to participate in her first recording session backing Sam Cooke. "You send me/ Summertime" was a national hit.

Carol fitted in perfectly and soon discovered studio-based session musicians were paid better than jobbing musicians and now divorced with two children to look after and also supporting her own mother, she welcomed the opportunity to play session guitar with what would become Gold Star Studios. She played acoustic rhythm guitar on Richie Valens' "Come On, Let's Go" and "La Bamba" (1958).

Carol had started to play a Fender Precision electric bass guitar and through Gold Star, found herself working with producer, Phil Spector She became one of a loose collective of elite musicians, initially known as "The Clique," in 1960. Working for demanding producers like Spectre and Quincy Jones The Clique could play any kind of music on demand. Carol Kaye was the lone female in the group which included: guitarist Glen Campbell (1936-2017), keyboardist Leon Russell (1942-2016), and drummers Hal Blaine (1929-2019), and Earl Palmer (1924-2008). Later Hal Blaine christened "The Clique" "Wrecking Crew." Individual members were able to pursue their own independent careers and in 1962, she released a surf single "Anitra's Twist"/"Ice Cream Rock." (GNP Crescendo label).

Her electric guitar can be heard on a number of hits between 1962 and 63 including: "Let's Dance" by Chris Montez, "Zip-A-Dee Doo-Dah" by Bob B. Soxx & The Blue Jeans', and "Da Doo Ron Ron" by the Crystals' among others

By 1963, Carol had become a regular session guitarist and when a bass player failed to turn up to a session at Capitol Records, she was asked to fill in. She loved playing bass and when Ray Pohlman left studio work to become a musical director, Carol Kaye became the most in-demand session bassist in Los Angeles and the hits kept on coming.

Her work with Phil Spector attracted the attention of other record producers and as her reputation grew, she was brought into sessions with many premier artists out with pop. Carol worked with Howlin' Wolf, Cannonball Adderley, Gene Ammons, Count Basie, and many others from different musical genres. She also worked at other studios including Western Recorders, Radio Recorders, CBS Studios, and RCA Victor Studios. The mid-sixties were a particularly busy time for the much in demand bass player and her contribution to pop music was well received with many hit records that defined the era. From the Beach Boys to Ike and Tina Turner to Nancy Sinatra and The Monkees her prominent bass playing can be heard.