The Last Unicorn soundtrack was recorded at De Lane Lea Studios in Wimbley, England in 1982. The album was released in Germany in 1983 by Virgin Records, but has not been released in the United States; it includes the film score's symphonic pieces. Mia Farrow's vocals, which appeared in the film, were overdubbed for the soundtrack album by Katie Irving.

The titular song is performed jointly by America and the London Symphony Orchestra, and plays in the film's opening credits while scenes from The Hunt of the Unicorn tapestries form a backdrop. It is referred to later as a leitmotif by the film score.

In his review for AllMusic, James Christopher Monger wrote:

The score itself, an appropriately somber and sentimental blend of fairy tale motifs and dark, Wagnerian cues, reflects the story's achingly beautiful tale of a unicorn who attempts to overthrow a maniacal king determined to rid the world of the magical creatures, while the songs are far more creative, daring, and eloquent than all of the cookie-cutter balladry that would eventually replace their type in future animated films. Like Watership Down, The Hobbit, and even Robert Altman's live action, Harry Nilsson-scored Popeye, this hard to find soundtrack is a gem from another age.

Kyle Anderson of the website Nerdist wrote that Jimmy Webb and America were among the "many great people [who] were involved" with the 1982 film, and that the album's "songs work pretty well".

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