Hexologic is a brilliant little logic puzzler, introducing nice mechanics along quite a comfortable difficulty curve, and Der Langrisser is a brilliant Warsong sequel that lets you choose multiple paths/alignments through the story.
I had a hard time choosing between Cho Aniki, Snail Maze, Phantasy Star, and Vib Ribbon for my final vote, but in the end I had to give it to the Snail Maze, because I remember being blown away as a kid that the game was built directly into the Master System hardware. And it's got a catchy tune.
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