LAUSR

Supported reducible oxides, such as indium oxide on monoclinic zirconia (In2O3/m‐ZrO2), are promising catalysts for green methanol synthesis via CO2 hydrogenation. Growing evidence suggests that dynamic restructuring under reaction conditions plays a crucial but poorly understood role in catalytic performance. To address this, the direct visualization of the state‐of‐the‐art In2O3/m‐ZrO2 catalyst under CO2 hydrogenation conditions (T = 553 K, P = 1.9 bar, CO2:H2 = 1:4) is pioneered using in situ scanning transmission electron microscopy (STEM), comparing its behavior to In2O3 on supports with similar (tetragonal, t‐ZrO2 or anatase TiO2) or lower (LSm‐ZrO2) surface areas. Complementary in situ infrared spectroscopy and catalytic tests confirm methanol formation under equivalent conditions. A machine‐learning‐based difference imaging approach differentiates and ranks restructuring patterns, revealing that partially reduced InOx species on m‐ZrO2 undergo cyclic aggregation‐redispersion via atomic surface migration, maintaining high active phase dispersion. High‐resolution ex situ STEM analysis further shows the epitaxial formation of In2O3 mono‐ and bilayers on (100) m‐ZrO2 facets, highlighting strong oxide‐support interactions. In contrast, sintering prevails on t‐ZrO2, a‐TiO2, and low‐surface m‐ZrO2, correlating with lower methanol productivity. This work underscores the pivotal role of oxide‐support interfacial interactions in the reaction‐induced restructuring of InOx species and establishes a framework for tracking nanoscale catalyst dynamics.