A Link To The Past: That game had a great feel for the ancient times of Hyrule. I always get a good feel when I play this game and I think it truly deserves a remake in TP/SS graphics.
However...
Majora's Mask was the best Zelda game by far. The game had such intense emotion for every single character. You couldn't meet a single person without wanting to know everything about them. From the simple life of the Postman to the love story of Anju and Kafei the game outdid the Zelda series. My favorite moment(s) of Majora's Mask has to do with any cutscene regarding the Song of Healing. Truly a masterpiece and I doubt I'll ever see another game up to par with Majora's Mask. I'd love to see a remake of this game as well, a mix of MM and TP graphics would be sweet!
I also still own the original soundtrack