Accelerating the migration of interfacial carriers ina heterojunctionis of paramount importance for driving high-performance photoelectricresponses. However, the inferior contact area and large resistanceat the interface limit the eventual photoelectric performance. Herein,we fabricated an S-scheme heterojunction involving a 2D/2D dual-metalloporphyrinmetal-organic framework with metal-center-regulated CuTCPP-(Cu)/CuTCPP-(Fe)through electrostatic self-assembly. The ultrathin nanosheet-likearchitectures reduce the carrier migration distance, while the similarporphyrin backbones promote reasonab...