LAUSR

Antimicrobial agents are massively used to disinfect the pathogen contaminated surfaces since the Corona Virus Disease 2019 (COVID‐19) outbreak. However, their defects of poor durability, strong irritation, and high environmental accumulation are exposed. Herein, a convenient strategy is developed to fabricate long‐lasting and target‐selective antimicrobial agent with the special hierarchical structure through bottom–up assembly of natural gallic acid with arginine surfactant. The assembly starts from rodlike micelles, further stacking into hexagonal columns and finally interpenetrating into spherical assemblies, which avoid explosive release of antimicrobial units. The assemblies show anti‐water washing and high adhesion on various surfaces; and thus, possess highly efficient and broad‐spectrum antimicrobial activities even after using up to eleven cycles. Both in vitro and in vivo experiments prove that the assemblies are highly selective in killing pathogens without generating toxicity. The excellent antimicrobial virtues well satisfy the increasing anti‐infection demands and the hierarchical assembly exhibits great potential as a clinical candidate.