Probably Super Mario World. It's the best 2D Mario, which is what you you think of as quintessential Mario gameplay. There's a reason there's so many romhacks for that one specifically. I played all the 2d marios except for the newest (Wonder).
For 3D Marios I don't have an opinion because I've only played Mario 64 and Mario Galaxy 2. Wonky Camera aside, I liked Mario 64 better because the movement feels really fun, even though Galaxy 2 has better levels.