The Xbox 360 Controller is an ABS plastic and gets prepared like any other plastic. The Controller is cleaned and scuffed, then washed with a plastic cleaner and sprayed with a plastic primer. It should be prepared the same way even if you chose to use an aerosol paint.
This video of how to paint an xbox 360 controller is geared to people whom already have a background in painting, obviously not a typical diy paint job.
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