Personally my favorite is Final Fantasy III, for a retro game soundtrack it's just amazing and the battle themes & overworld theme are some of the best in the series.
Easily the Silver Surfer soundtrack. It has such an intense arrangement that not only delivers a very high pace to the otherwise frustratingly hard game, but also emphasizes the futuristic nature of the overall story!
Also, Battletoads! Catchy as hell, pumping and awesome, even the pause tune was cool!
"I'll take a potato chip... AND EAT IT!"
Light Yagami, Death Note
"Ah, the Breakfast Club soundtrack! I can't wait 'til I'm old enough to feel ways about stuff!"
Phillip J. Fry, Futurama
The first Castlevania also had a good overall soundtrack but Bloody Tears is one of my favorite songs on the NES ever. Mega Man 2 as a whole had one of the best soundtracks too, and I second SMB3.
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Topic: Best NES Soundtrack?
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