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You selected the issue: Test the Steam Overlay

The Steam Overlay is vital to Steam Controller functionality. Press the Steam button on your controller, or SHIFT+TAB on your keyboard to produce the overlay. If the Steam Overlay doesn't appear, make sure you've enabled it through the Steam settings menu.

Steam may have issues applying the Steam Overlay to a non-Steam or retail game if it hasn't been added to your Steam library, particularly when the game has its own launcher.