The first recording featuring Moog Synthesizer - The Zodiac: Cosmic Sounds (1967) ?

video by George Greene

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"The Zodiac: Cosmic Sounds was a collaborative concept album on the theme of the signs of the Zodiac. It was issued by Elektra Records in May 1967 and featured early use of the Moog synthesizer by Paul Beaver, with music written by Mort Garson, words by Jacques Wilson, and narration by Cyrus Faryar. The Moog Modular synthseizer has a prominent role on the album. Rather than being limited to just spooky sounds, Beaver contributed a veritable clinic of fundamental Moog modulations, from soothing melodies and textures to sharply percussive interactions with the other session musicians. 'Must be played in the dark,' are the instructions printed in purple on the back of album cover. Although the Moog Synthesizer is not mentioned in the liner notes Paul Beaver is credited vaguely with 'electronic instruments'. This was not only the first commercial release of a record featuring the Moog but also the first to chart, spending a total of nine weeks on the Billboard album chart."

If you know of anything earlier, feel free to leave a comment. Surprised there is no mention of this release on Wikipedia's article on the Moog Synthesizer, but there is a separate article on the release here. Wikipedia also mentions use of the Moog on The Monkey's 1967 release of Pisces, Aquarius, Capricorn & Jones Ltd, recorded April–October and released in November. The Zodiac was rleased in May of 1967.