[en] Highlights: • Hierarchical assembly, Fe doping and Ag loading are used to design ZnO catalyst. • Novel Platycladus orientalis–shaped Ag/Fe-doped ZnO heterostructure is synthesized. • Photocatalytic mechanism promoted synergetically by Fe doping and Ag loading is proposed. • Ag/Fe-doped ZnO exhibited excellent photocatalytic activity and cyclic stability. -- Abstract: The Ag/Fe-doped ZnO composites were designed by controllable intergration of the three strategies of hierarchical assembly, Fe doping, and Ag loading. The 3D Fe-doped ZnO hierarchical nanoflowers were firstly constructed with Platycladus orientalis–shaped petals via a hydrothermal method, and then Ag nanoparticles were anchored on the surface of Fe-doped ZnO nanoflowers through impregnation/reduction of silver nitrate solution. The samples were characterized by using XRD, SEM, TEM, HRTEM, XPS, Raman spectra, BET, UV–vis DRS, PL, EIS, Mott-Schottky plots, and photocurrent response. The results showed that Fe doping increased BET surface area and oxygen vacancies of ZnO, Ag loading produced the LSP absorption at ~530 nm, Fe doping and Ag loading together extended the visible light absorption and facilitated the separation of photogenerated carriers, which favors photocatalytic activity of ZnO. The maximum degradation efficiency of 92.3% for MO was achieved after visible light irradiation for 80 min when the feed atom ratio of Fe to Zn was 1.2% and Ag loading was 4 wt% of Fe-doped ZnO. Four cycle tests had little effect on the morphology and structure of Ag/Fe-doped ZnO, suggesting good cycling stability. The photocatalytic mechanism was elucidated based on the scavenger experiments and energy bands alignment.