Octave Doctors And The Crystal Machine, Tim Blake's short solo track on Gong's Flying Teapot album, was done with a VCS-3. And the sequencer thing on Pink Floyd's On The Run was done on a Synthi-AKS (not exactly melodic but the instrument is playing actual tuned notes).
Though Del Dettmar used his Synthi A to make "outer space blips and bleeps", there were occasions where he'd play something melodic, like on 7x7. And it's the Synthi A playing the ring modulator bells at the beginning of Tangerine Dream's Rubycon album.
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