I've written rhapsodically here about No More Heroes and why I admire the game so much. Oddly - I have no idea why - I never mentioned the music in the game. This is a huge oversight because Masafumi Takada's score and sound design play a big role in the experience delivered by NMH. Takada's compositions for the ten ranked assassins are especially notable because each boss is a distinctive twisted personality requiring a unique musical signature.
So to right past wrongs I will recommend an interesting interview with Takada at Gamasutra. Takada talks about his work at Grasshopper on NMH, Killer 7, and several other games, as well as his collaboration with designer Suda 51.
I was astounded to learn that Takada has no studio and does all of his composing and sound design at a desk in his office situated among other departments.
If you feel something different about the audio in the Grasshopper games, it's probably because the audio department is on the floor where everyone else is -- together with the graphic, project management, planning and programming departments, so the audio staff is producing work in an environment where they can easily communicate with the rest of the production team. That can take the project in a good direction.
You can read the complete interview here.