From my cart collection, not released:
SNES/SFC
Legend of the Mystical Ninja
Mario and Wario, Nintendo's best puzzle game ever
ActRaiser 2
Aerobiz
Aerobiz Supersonic
Big Sky Trooper
Captain Commando
Captain Novolin
Chrono Trigger
Clue!
Darius Twin
Dino City
Doom
Drakkhen
Earthbound
Final Fantasy Mystic Quest
Final Fantasy III/VI
Hit the Ice
Illusion of Gaia
Joe and Mac
Knights of the Round
Lagoon
Lord of the Rings
Mario is Missing
Mario's Time Machine
Math Blaster
Mega Man X
Monopoly
Mortal Kombat
Mortal Kombat 2
Pac-Man 2
Phantom 2040
Q-Bert 3
Rex Ronan
Robotrek
SOS
Shaq Fu
SimEarth (SNES)
Skyblazer
Spanky's Quest
Star Fox
Star Trek Starfleet Academy
Super Mario All Stars
Super Mario World 2: Yoshi's Island
Super Widget
Thomas the Tank
Uniracers
NES
Bucky O'Hare
Dr. Mario
Dragon Warrior
DuckTales
Faxanadu
MC Kids
Rampage
Snoopy's Sports
Where's Waldo
Yo! Noid
N64
Blast Corps
Conker's Bad Fur Day
Goldeneye 007
Mischief Makers
Pokemon Stadium
Star Wars Rogue Squadron
Star Wars SOTE
Genesis
Aladdin
I don't really own a lot of carts, but just looking at the stuff I own alone there's no shortage of games that would be great on the service and aren't there yet, even categorically excluding licensed games.
Just off the top of my head, the following games I don't own and would want on VC:
Adventures of 3d World-Runner (NES)
Chip 'n' Dale Rescue Rangers 1/2 (NES)
Crystalis (NES)
DuckTales 2 (NES)
The Guardian Legend (NES)
Doom 64 (N64)
Mission: Impossible (N64)
Pilotwings 64 (N64)
EVO: The Search for Eden (SNES)
Goof Troop (SNES)
Hook (SNES)
Secret of Evermore (SNES)
Soul Blazer (SNES)
Sunset Riders (SNES)
Terranigma (Euro SNES)
Turtles in Time (SNES)
Twisted Tales of Spike McFang (SNES)
So, no, if we're asking them to actually make an effort on this stuff, they're not even close to done.