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Castlevania III Ninja Gaiden 3 Super Mario Bros. 3 Blaster Master Mega Man 5
I know, generic answers... I also like Magic of Scheherazade, Legacy of the Wizard, Dragon Warrior 4, and Little Samson. And of course, the Mega Mans / Castlevanias / Ninja Gaidens always look good. I also have a soft spot for Battletoads.
Use your computer mouse to navigate the internets. Be sure to talk to everyone you meet. You're sure to gain lots of valuable information.
There's... really a lot of good looking NES games. From the smoothly animated (Metal Storm, Kickmaster, Moon Crystal) to the cinema-heavy (Ninja Gaiden, Choujin Sentai Jetman, Deja Vu). Totally Rad even gets a nod for having both.
The Dragon Warrior games fall handily into this; the 1st game has lush backdrops and huge enemies, the 2nd has that amazing fade-in introduction, the 3rd has the storyline introduction, the 4th has an animated multipart final boss...