Abstract

In this paper, we intercalated 5,10,15,20-tetra(4-carboxyphenyl)porphine (TCPP) into layered double hydroxides (LDHs), where tilted J-type aggregation extends light absorption to the UV-vis-NIR range and introduces a synergistic photothermal effect. High-energy photons drive electron–hole separation for two-electron O2 reduction to *OOH and H2O2, while low-energy photons generate localized heat to enhance charge separation and lower barriers. The ordered ‒COOH/‒NH groups further adsorb and stabilize *OOH intermediates via hydrogen bonding, enabling efficient and selective H2O2 synthesis under solar light.