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I enjoy using Keyboard Maestro to set custom keys to take control of apps, I can apply more functions to the play/pause button in the earphone remote, but by default it is set to control iTunes.

How to disable or overwrite the default setting of these button?

I'm using a Mac, and use the iPhone earphone with remote

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Can you clarify your question a little? I am unsure whether you are using an iOS device, or just your iOS headphones on you Mac. –  stuffe Oct 20 '11 at 11:48
    
@stuffe I'm using mac, and use the iPhone earphone with remote –  mko Oct 20 '11 at 11:55
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Not providing this as an answer, as I do not know if it will work (not at a Mac and cannot test) but whatever F key the play/pause key is on your Mac (they move around, depending on age, mine is F8), you could try to reassign that, and see if it also changes your headphone command. This is just to check if they are linked, it may be that the headphone is just sending an F8 command etc. If it does, then that's your answer, although this also changes the key and that may not be suitable, if it doesn't, then I would tentatively say it's not possible. –  stuffe Oct 20 '11 at 11:58
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