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Electronic and ionic conductivity of an oxide overlayer can dictate the active site location, which can increase OER selectivity over competing reactions. 

Unbiased photoelectrochemical hydrogen production with high efficiency and durability is highly desired for solar energy storage. Here, we report a microbial photoelectrochemical (MPEC) system that demonstrated superior performance when equipped with bioanodes and black silicon photocathode with a unique “Swiss-cheese” interface. The MPEC utilizes the chemical energy embedded in wastewater organics to boost solar H 2 production, which overcomes barriers on anode H 2 O oxidation. Without any bias, the MPEC generates a record photocurrent (up to 23 mA cm −2 ) and retains prolonged stability for over 90 hours with high Faradaic efficiency (96–99%). The calculated turnover number for MoS x catalyst during a 90 h period is 495 471 with an average frequency of 1.53 s −1 . The system replaced pure water on the anode with actual wastewater and achieved waste organic removal up to 16 kg COD m −2 photocathode per day. Cost credits from concurrent wastewater treatment and low-cost design make photoelectrochemical H 2 production practical for the first time.