That wasn't Fay Presto with a kitchen sink and garden hose was it? She/He was scary to me even as a child.
If not then the Theremin was used a lot in the older horror films but let's not forget The Beach Boys 'Good Vibrations'.
[ame=http://uk.youtube.com/watch?v=cd4jvtAr8JM]YouTube - Theremin Lesson One[/ame]
For me the Ondes Martenot just beats it because it has can have an optional beater sound unit, like someone hitting spoons very fast mixed with the sliding whistle sound. That turns up in The Quiller Memorandum theme at the start when the guy is walking along the street and is introduced at 1:00 in the video below.
[ame=http://uk.youtube.com/watch?v=LZSEGZ66_O8]YouTube - The Quiller Memorandum (1966)[/ame]

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