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To me there is no real doubt: Super Mario Bros. 3. That game has so much charm and creativity. Extremely polished with a perfect level of difficulty. I still replay that game every few years and get immersed each time. I still love replaying Super Mario 64 as well, but with time the flaws have become more obvious (still a masterpiece though), Super Mario World doesn't do much for me anymore.
SMB3 is certainly the best 2D Mario game of all time, probably the greatest Mario game period, and a serious contender for greatest game of all time. Oh, and in contrast to popular belief, the NES version is the go-to version, not the SNES All-Star version. The 16-bit update completely ruined the charm of the 8-bit graphics.

The other 80's game that is an absolute masterpiece is of course Mega Man 2. They pretty much perfected the gameplay with that one. Certainly the best balanced in the series and the one with the greatest sound track, of any NES game really.

Some other strong contenders:
3. Ninja Gaiden
4. The Legend of Zelda
5. Super Mario Bros.
6. Galaga
7. Tetris
8. Donkey Kong
9. R.C. Pro-Am
10. Ms. Pacman