It depends. Are we talking about just titles available on the system at launch, or killer apps intended to sell the platform?
Best title available at launch was Breath of the Wild, hands down.
But if we're talking about killer apps that forced you to purchase the system, then both of the Zelda games on your poll would get knocked off. If we're talking about it from that angle, I'd say it's a three way tie:
Super Mario World for perfecting the sidescrolling formula, Halo for the introduction of recovering health in FPS games, and Mario 64 for show the world how a platformer should play when there's a Z-axis.
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