A link to the Past in terms of 2D - It was everything I loved from the original zelda increased 10 fold and more.
Majora's Mask In terms of 3D - It was everything I loved about ocarina of time only fleshed out a lot more. I sometimes feel like OOT was the test and MM was the real game.
Also up there is Zelda 2 for me, I always am surprised when people complain about the difficulty of this game, the only annoyance to me is that it sends you back to the beginning each time you die but I mean... I've been beating this game since I was 5. I find it way easier than most Megaman games. Difficulty should not be a complaint, this is why most modern day games are for pussies. It should be if the ends justify the means. Most NES era games grew from arcade games and so brought over alot of the difficulty. I see no reason to play a game unless it is challenging me in some way.
Mostly I love the style of the world in this game though. I would love to see a new Zelda that took place in the world that Zelda 1 and 2 were situated in. I miss the weird meld of Roman and medieval architecture.