The Dillards — Doug and Rodney Dillard, Dean Webb, and Mitch Jayne — were from Salem, Missouri, and relocated to Los Angeles in the early 1960s, where they became part of the folk revival scene centered on the clubs and coffeehouses of the Sunset Strip. Their Elektra Records albums placed them within the urban folk movement while their Missouri roots and bluegrass instrumentation gave them a credibility as bearers of an inherited tradition that distinguished them from many of their contemporaries. Their recurring appearances on The Andy Griffith Show as the Darling family brought their music to a television audience that dwarfed any folk club's capacity.

By the time they recorded "The Last Thing on My Mind" / "Lemon Chimes" for Capitol Records (Capitol 5524), released in 1965, the Dillards were operating in a commercial landscape that was beginning to shift away from the strict acoustic folk sound toward the electric folk-rock that would come to dominate in 1966 and 1967. Tom Paxton's "The Last Thing on My Mind" had become one of the folk revival's most covered songs, and the Dillards' version placed them in dialogue with the broader repertoire that the revival was drawing on and disseminating.

The Capitol single represents a transitional moment in their career — between their Elektra folk-bluegrass period and the more explicitly rock-influenced direction they would pursue in the late 1960s with the group Dillard and Clark. The Dillards' contribution to the folk-rock synthesis of the mid-1960s has been documented by music historians as significant, and their Capitol recordings occupy a specific place in that transition.

Session details drawn in part from the Bluegrass Discography.