Riding high on the success of these singles, Donovan planned an album consisting of stripped-down acoustic children's music inspired by his spring 1967 move to Buck's Alley Cottage in Hertfordshire, where he had been writing songs celebrating its natural beauty.

[4] When he proposed the album to producer Mickie Most that August, Most did not find the project viable, which led to a temporary parting of ways between the two.

Other songs included "Voyage into the Golden Screen", written on the same spring 1966 trip to Mexico that had produced "Sand and Foam"; "Isle of Islay", penned on a summer 1966 trip to the Scottish isle of its title following his drug bust; "The Tinker and The Crab", first introduced during concerts in late 1966 and announced as the singer's next single in a March 1967 issue of New Musical Express, although this plan was scrapped;[5] and "Lay of the Last Tinker", performed along with the previous three songs at the singer's acclaimed Royal Albert Hall show in January 1967.

"Wear Your Love Like Heaven" eventually gave the "for adults" disc its title and was released as the album's lead single in America.

Several of his earlier records had contained both veiled and open references to drug use (particularly marijuana and LSD), but since the release of Mellow Yellow, he had both been arrested and prosecuted for marijuana possession, and had seen people he knew turning to harder drugs (speed, heroin, cocaine), and bemoaned the damage this caused in their lives.

A Gift From a Flower to a Garden appeared in an elaborate box set package which included both discs, along with a series of 12 A4 sheets of special coloured paper with drawings by friends Mick Taylor and Sheena McCall illustrating the lyrics to the songs on the children's record.

[4] The front cover photo design of the album features a Pre-Raphaelite style infrared photograph (requiring seven colour separations for printing, instead of the usual four) of Donovan posing by the cliffs of Cornwall in a full robe and makeup, holding flowers in one hand and peacock feathers in another.

[16] In the US, Billboard opined "his poetry, clipped lamenting voice and and fable-like simplicity are hypnotic" while Cashbox hailed the album as "a feast for the eyes in spectacular packaging, ears in delicate and moving songs, and mind through tantalizing lyrics and melodic weavings".

[17][18] Retrospectively, AllMusic stated that the album "stands out as a prime artifact of the flower-power era that produced it," and noted that while "the music still seems a bit fey … the sheer range of subjects and influences make this a surprisingly rewarding work.

[14] The Quietus noted of For Little Ones that "the words aren’t patronising, dumbed down, or tailored to what adult writers think children either want to hear or should be told...The music is gentle enough for the album to work as a collection of lullabies, but the main reason these are songs aimed at "the dawning generation" is that they take the form of fables and fairy tales, of the kind common to both the 19th century folk revival and the Victorian children’s literature of the same period: a canon with a unique combination of faded innocence and haunted strangeness that the psychedelic songwriters of the 60s saw as a rich well to draw from.