"Little Wing" emerged during late 1967 as Hendrix and his band expanded their sonic palette toward psychedelia, with recording sessions at Olympic Studios involving multiple guitar effects—unconventional pickup positions, Leslie speaker modulation, and various overdubs. The song's surrealist lyrics and transportive arrangements reflected Hendrix's ambition to capture the experimental atmosphere of the era.

The track's most iconic feature arose unexpectedly when Hendrix located a leftover glockenspiel during overdub sessions and quickly recognised its potential. Working with engineer Eddie Kramer, Hendrix recorded striking bell tones that, enhanced by studio reverb, created the shimmering metallophone texture that became the song's defining characteristic. This acoustic instrument's integration proved central to "Little Wing"'s enduring status as a psychedelic landmark.