No he didn't. Black is Black was recorded by Spanish group Los Bravos.
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Gary Lewis recorded a version of this song on his " This Diamond Ring" LP - Gene Pitney never recorded this song. The hit version is by Bobby Vee
http://www.whosdatedwho.com/music/songs/gene-simmons.htm
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Long Black Veil
The song It's a Heartache, was never used in a movie. It was made popular by Bonnie Tyler and was a US hit in 1978. It was also recorded by Juice Newton, Rod Stewart, Ronnie Spector, and Gene Pitney.