Developing the catalysts for methanol steam reforming (MSR) via interfacial construction still remains many challenges. In this study, the effects of ZnO content on the performance of ZnyCe1Zr9Ox were studied for MSR. The best-performing ZnyCe1Zr9Ox catalyst exhibited full methanol conversion and higher H-2 production rate of 0.31 mol.h(-1).g(c)(at)(-1) 400 degrees C. Characterization results revealed the synergistic effect among ZnO, CeO2 and ZrO2 after forming a solid solution and the incorporation of Zn2+ into Ce1Zr9Ox matrix not only modulate the ratio of surface O-Latt/O-Ads, but also generate new Zn-O-Zr interfacial structure corresponding to the lattice/bridge oxygen to increase the selectivity of CO2. The excess oxygen vacancies on the samples surface favor the decomposition of methanol to generate the undesired CO. This study proposes a new design strategy for developing highly efficient composite MSR catalysts by control of the lattice/bridge oxygen and surface oxygen vacancy. (C) 2020 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.