A few that I really enjoyed:
Perhaps not the best games but Dragon's Lair and Space Ace on the SNES were completely unique from their arcade versions.
Doom & Wolfenstein 3D - while not exact ports from the PC were the versions I played first.
Gradius III (while not the most overlooked is one of my favorite shooters on SNES.
Knights of the Round - Basically Final Fight set in King Arthur's world - and you actually play as Arthur, Lancelot and a 3rd character Percival. - as you play, armor and weapon are improved.
Mechwarrior 3050 - a unique overhead version of the PC game. Rock & Roll Racing - racing + combat + licensed rock music made this game memorable.
Super Pinball: Behind the Mask is one of my favorite pinball games - this one was unique for the time period as the table view was full 3D.
Top Gear / Top Gear 2 - these games have some of the best music on the system - or at the very least some of the best for racing games on it. - Top Gear 3000 was ok, but I didn't have as much fun with it as the first 2.
I also have to recommend the previously mentioned Sunset Riders - it's not only as much fun as Turtles in Time - it's also a lot more arcade accurate than the version on Genesis.
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