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If you really need to use the Caps Lock key, there's a way to change the search key into a Caps Lock key in the settings. Unfortunately, this is time consuming, especially if you constantly switch between the search key and the Caps Lock key. There's a better way: press both Shift keys at the same time to enable or disable Caps Lock. It's an undocumented shortcut that works in the latest versions of Chrome OS.
{ Thanks, Cougar. }