I can’t believe Dylan’s Slow Train Coming, Saved, and Shot Of Love haven’t already been mentioned.
Aretha Franklin: Songs Of Faith. Recorded in 1956 in a Baptist church in Detroit (Aretha was 14 years old!), originally released on J-V-B Records, rereleased in ’65 (with extra tracks) in ’65 on Checker Records.
Larry Norman was a very well-known figure in the Christian Rock movement (and may still be). He made a bunch of albums, and if his name sounds familiar (unless you’re from San Jose or are a Rock historian, I doubt it ;-), he was one of the two lead singers in the 1960’s 1-hit wonder group People, known for their cover of The Zombies "I Love You".
Ritchie Furay of Buffalo Springfield and Poco also went Christian, making a fair number of albums for the Christian Rock market.
Almost all the music composed by J.S. Bach is of a spiritual nature, much of it written to be performed at his day job, a church organist.