No, I'd rather they continue working on GameBoy games, move on to GBA games, and eventually start getting DS games up there. Making NES games available is getting sidetracked enough as it is, and getting SNES games up there would be pointless in my opinion, but I wouldn't really complain about being able to play Super Metroid on the go.
The big problem with N64 games on 3DS is the buttons. One analog, one d-pad, six face buttons, and three triggers/shoulder buttons won't translate well to one analog, one d-pad, four face buttons, and two triggers/shoulders. You could use the touch screen as a substitute for some of those functions, but that would require significantly more effort; after all, no current VC titles employ the touch screen as anything other than a freeze-state menu. Even if you mapped both the L and Z N64 buttons to the 3DS's 'L' button -- which might work -- there would still be two face buttons unaccounted for.
