Donovan's Greatest Hits is a distinct entry in Donovan's discography for several reasons. First, it collects three singles that were previously unreleased on any album: "Epistle to Dippy"; "There Is a Mountain"; and "Laléna." It also presents the unedited "Sunshine Superman" (one minute and fifteen seconds longer than the original 1966 single and LP release), and most of the songs appear for the first time in stereo. Lastly, Donovan's Greatest Hits contains re-recordings of "Catch the Wind" and "Colours" with Big Jim Sullivan playing guitar, John Paul Jones on bass and keyboards and Clem Cattini on drums. Epic Records could not obtain the right to release the original recordings of these two songs, so Donovan recorded new versions in May 1968 with a full backing band and a lavish production by Mickie Most.

Donovan's Greatest Hits marked the high point of Donovan's popularity in both the United States and United Kingdom. It also most likely had the effect of keeping many of Donovan's recordings on the shelf to avoid oversaturating the market. Nearly all of Donovan's next studio album was already recorded by the time of this release but remained unreleased until August 1969.

Interesting and beautiful songs, surprisingly varied. Donovan's interest in music always extended well beyond the genres with which many casual listeners may have associated him since the 1960s, and a listen to this collection of his hits from that early era of popular success reveals much of his breadth. A most enjoyable journey through one talented Scotsman's musical imagination.