Along with influential work with Booker T & The MG's, Cropper co-wrote "Knock on Wood" with Eddie Floyd, "In the Midnight Hour" with Wilson Pickett and "(Sittin' On) The Dock of the Bay" with Otis Redding. In 1969, Cropper released his first solo album, With a Little Help From My Friends.
When Cropper left Stax in the fall of 1970, the label lost one of its most successful producers and songwriters. Cropper then set up TMI Studios with Jerry Williams and former Mar-Key Ronnie Stoots. There he played guitar and produced various Musicians including Tower of Power, Rod Stewart, John Prine, José Feliciano, The Jeff Beck Group, Ringo Starr and John Lennon. It's little-known that Cropper also played guitar on the cover of The Velvet Underground's "Femme Fatale" that appears on fellow Memphians Big Star's Third/Sister Lovers.
By 1975, Cropper had moved to Los Angeles and along with Jones, Jackson and Dunn, reformed Booker T. & the M.G's. Jackson, whom Cropper called "the greatest Drummer to ever walk the earth," was murdered in his Memphis home before the group could make their comeback. In 1978, Cropper and Dunn became members of Levon Helm's RCO All-Stars, and then went on to figure prominently in the Blues Brothers Band with the Drummer Willie Hall. This led to two albums and two movie soundtracks. Cropper also re-recorded "(Sittin' On) The Dock of the Bay" (1979) for Sammy Hagar. Cropper lived in Los Angeles for the next thirteen years before moving to Nashville and reuniting with the Blues Brothers Band in 1988.
Cropper has a cameo in the "Weird Al" Yankovic mockumentary The Compleat Al (1985), where he plays a bit of "Soul Man" in an unsuccessful attempt to join Al's band.
In 1992, Booker T. & the M.G.'s were inducted into the Rock and Roll Hall of Fame, and Cropper appeared with a new line-up of the group for the Bob Dylan 30th Anniversary concert, on October 1992 at Madison Square Garden, performing songs by and backing Dylan, Eric Clapton, George Harrison, Tom Petty, Johnny Cash, Chrissie Hynde, Sinéad O'Connor, Stevie Wonder and Neil Young. The concert was recorded and later released as The 30th Anniversary Concert Celebration (1993). Young later recruited this line up of Booker T. and the M.G's, to tour with him and record as his studio band.
In 1996, Cropper was named "the greatest living guitar player" by Britain's Mojo magazine. When asked what he thought of Cropper, the Guitarist Keith Richards said, "Perfect, man." In February 1998, Cropper released Play It, Steve! which included some of soul music's most enduring songs. The album title came from the "shout" of the title phrase by Moore on Sam & Dave's "Soul Man," and later by John Belushi (with the Blues Brothers).
In June 2004, Cropper appeared with Dunn and Jones as the backing band for Eric Clapton's Crossroads Guitar Festival, held at the Cotton Bowl in Dallas. Others who appeared included Joe Walsh and David Hidalgo. On June 9, 2005, Cropper was inducted into the Songwriters Hall of Fame.
He co-produced The Memphis Album (2007), recorded by Australian soul singer Guy Sebastian. Cropper also played guitar on the following promotional tour, which was recorded and released two years later as The Memphis Tour. On March 2, 2008 Cropper and Sebastian were guests on the Vega Sunday Session with host Mark Gable from the rock band the Choirboys. On July 29, 2008, Cropper and Felix Cavaliere released the album Nudge It Up A Notch. In August 2008, Cropper appeared at the Rhythm Festival alongside the Animals.
On November 12, 2009, EMP/SFM presented Cropper with their "Founders Award." On October 17, 2010, Cropper was inducted into the Nashville Songwriters Hall of Fame.
On August 9, 2011, Cropper released the album Dedicated which was his tribute to the "5" Royales. In 2013 he was a special guest at selected concerts as part of Peter Frampton's Guitar Circus Tour, including the first performance which featured Frampton, Robert Cray and Vince Gill.
In April 2013, Cropper appeared with Jones and Matt Guitar Murphy as Booker T and the M.G.'s at Eric Clapton's 4th Crossroads Guitar Festival at Madison Square Garden in New York City.