For me the NES dogbone controller wins. It was a 100% improvement on the box NES controller. And the precursor of the SNES and future Nintendo controllers. I actually owned one back in the day and after using it, I never went back to the NES box controller again.
Runner up goes to the Wii U gamepad. For a TV based controller is it unreasonably large and heavy. And not so suitable. But for off TV game playing it is near perfect. You can rest the gamepad on yourself or a deck or something as you play so it's weight is not an issue for extended periods of play. You can also do this for TV play but it just doesn't work as well.