LAUSR

Photo(electro)catalysis methods have drawn significant attention for efficient, energy‐saving, and environmental‐friendly organic contaminant degradation in wastewater. However, conventional oxide‐based powder photocatalysts are limited to UV‐light absorption and are unfavorable in the subsequent postseparation process. In this paper, a large‐area crystalline‐semiconductor nitride membrane with a distinct nanoporous surface is fabricated, which can be scaled up to a full wafer and easily retrieved after photodegradation. The unique nanoporous surface enhances broadband light absorption, provides abundant reactive sites, and promotes the dye‐molecule reaction with adsorbed hydroxyl radicals on the surface. The superior electric contact between the nickel bottom layer and nitride membrane facilitates swift charge carrier transportation. In laboratory tests, the nanostructure membrane can degrade 93% of the dye in 6 h under illumination with a small applied bias (0.5 V vs Ag/AgCl). Furthermore, a 2 inch diameter wafer‐scale membrane is deployed in a rooftop test under natural sunlight. The membrane operates stably for seven cycles (over 50 h) with an outstanding dye degradation efficiency (>92%) and satisfied average total organic carbon removal rate (≈50%) in each cycle. This demonstration thus opens the pathway toward the production of nanostructured semiconductor layers for large‐scale and practical wastewater treatment using natural sunlight.