Decoupling Interlayer Interactions Boosts Charge Separation in Covalent Organic Frameworks for High‐Efficiency Photocatalytic CO2 Reduction

with 94% selectivity under visible light irradiation without additional photosensitizers or co-catalysts. These findings establish interlayer engineering as a crucial design principle for developing high-performance COF-based photocatalysts for solar energy conversion applications.