Note: MotioninJoy is somewhat unsafe regarding how it operates - needing an internet connection and will display ads (which can maybe display unwanted content) and uses unsigned drivers (this is fine). This page will cover setting up MotioninJoy to pair your DS3 controller to the PSP Go and using Better DS3 to mange what your DS3 controller is paired to. If you don't have a PS3 there is a way to do it on the computer using MotioninJoy.
The easiest method to connecting your PS3 controller to the device is by using a PS3 console and following the on-screen instructions on the PSP system.
Using MotioninJoy and Pairing your Devices:.