No More Heroes: Desperate Struggle has no MotionPlus enhancements but it does support the Classic Controller. The info comes via 1UP:
As it turns out, Grasshopper’s motivation for this had less to do with the mingames and more to do with the popularity of Capcom’s Monster Hunter Tri, which many people in Japan play using the Classic Controller (and was even packaged at the same time as the Classic Controller Pro). According to Suda, Grasshopper — and Japanese publisher Marvelous — wanted to support this controller to appeal to those players.
I wonder if that was really the only reason. Combine this with Suda’s love for the 360 and well…really, I don’t see any way these ports are not happening. Retrofitting the first game with traditional controls wouldn’t be very difficult. This is further indication that No More Heroes could very well be at the top of MMV’s to-port list.