that happened to my 2001 C320, I had to pull down the switch, disconnect the switch from power and the sunroof motor from power. then reconnect them, and hold the button closed for five seconds, then open the sunroof all the way and hold thee button open for a few seconds, and the same goes for the tilt option, that should synch the sunroof..

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2001 Mercedes-Benz C320 3.2
1991 Mercedes-Benz 300E 3.0