The title of the "You Bet Your Life" theme was "Blues for Jaws," referring to Eddie "Lockjaw" Davis, who gave Shirley her big break and made her the co-leader of his band (complete with Liberace-ish candelabra on top of her Hammond and lights on the bass pedals to show off her feet). Since her recording in the last years of her life was sporadic (and mostly on piano), I don't know if this song is available on commercial CD.
You can't go wrong with most of her albums, but I recommend any Prestige release, when she was at her peak. In particular, go for "The Trio Sessions, Vol. 1," her first recordings as a solo act--it's just her, a bass player and a dummer and it grooves from start to finish (except for a version of "Brazil" that sounded like it was recorded to be released as a single and get MOR airplay backtimed into news).