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You can screenshot anytime as long as Steam is running by holding the Xbox Guide button and pressing a certain button. To check what button that is, from Gaming Mode, hold the Xbox Guide button for a few seconds. A list should pop up showing all the commands, Take Screenshot should be the last one.
To change that, go to Settings -> Controller -> Guide Button Chord Layout. Edit Layout, find your button, give it a new command, tab over to System, and choose Take Screenshot. Back out, select the cogwheel to the left of "Edit Layout" and Export Layout.
If you want to screenshot from the desktop, change the Desktop Layout instead.
Just use the Guide Button shortcut.
Thanks for the guide, it really help a lot