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I do mean stop, not pause. If one navigates to, say, the iTunes Store, the Pause button changes to Stop, but I want something that always works no matter my location in iTunes.

Workarounds (such as AppleScript) are acceptable as long as they aren't too difficult to set up.

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up vote 4 down vote accepted

The AppleScript for this is pretty simple:

tell application "iTunes" to stop

You can make this easily accessible by creating a Service.

Open Automator and create a new document. Select the Service document type. Set the Service receives: menu to no input. Drag in a Run AppleScript module and paste that code into its text box. Save the service and give it a name.

You'll now be able to activate it by going to the current app's menu and choosing Services-> Stop iTunes (or whatever you named the service).

You can assign a keyboard shortcut by going to System Preferences-> Keyboard-> Services, finding the service (it should be under General at the bottom) and adding a shortcut.

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In Applescript, the script tell app "iTunes" to stop should work.

And the pause button is only available in the currently playing playlist; anywhere else, it will be stop.

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Hold the Option key down, while clicking the Pause button.

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You can't! What I do is either "Quit iTunes" or delete the tract (I only delete if I already have the song on a DVD; I can add it back to my library at a later date).

iTunes is not user friendly. I use it sparingly.

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Your answer is utterly false. Since time of asking (at which point even then your answer was incorrect), iTunes now lets one stop playback with command-period or the respective menu item. – timothymh Jul 31 '14 at 2:19

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