The line-up at the time officially consisted of Neil Young, Stephen Stills, Richie Furay, Dewey Martin, Bruce Palmer, and Jim Messina, though the band itself was essentially broken up and the album was put together from previous recordings, some made up to a year earlier.

Jim Messina acted as the album producer and mixing engineer, with input from Furay, as the two compiled the record to fulfil the band's last contractual obligation to its label.

By the time this album was released, the members were already involved in their next projects: Richie Furay, Jim Messina, and Rusty Young were busy forming the country-rock band Poco, Stephen Stills was forming Crosby, Stills & Nash, and Neil Young was performing with a group known as The Rockets which would later become the band Crazy Horse.

His face is shown on the back cover photo montage with a humorous, partially obscured, "mad" sign aligned, due to Palmer resembling Alfred E. Neuman in the shot.

Barry Gifford of Rolling Stone called Last Time Around Buffalo Springfield's "most beautiful record" and "a final testament to their multi-talent".

[3] Robert Christgau, writing for Esquire, called it a "beautiful farewell album" of "countrified music", in which "country elements are incorporated into a total style".