OSX keyboard shortcuts for iTunes from outside the application

If you have an Apple keyboard, F8 (or fn-F8) should start or pause playback. If you don't, you might be able to use KeyRemap4MacBook to remap other key combinations to the special F-keys.

Alfred also has some keywords for controlling iTunes, like play and next. You can assign shortcts to them by creating a workflow:

You could also assign a shortcut to a script like this:

tell application "iTunes"
    if player state is playing then
        pause
    else
        play
    end if
end tell

I use scripts like this to jump forward and backward:

try
    tell application "iTunes"
        set player position to player position + 30
    end tell
end try

One simple solution, if you don't have a keyboard with shortcuts, is to set the miniplayer to always stay on top of other windows for a fast click.

Note: Stackoverflow won't let me post pictures of this because my reputation is too low, but it works for me :)