For industrial catalysis, a simple and green process for catalyst synthesis has always been pursued. In this regard, we utilized NaCl, one of the most common salts, as a template to prepare transitional metal oxide catalysts with both abundant porosity and well-dispersed noble metal species. Interestingly, this dispersion by NaCl was realized by solid-state grinding. Importantly, those catalysts afforded excellent performance in redox processes.

Doped Ceria with abundant oxygen vacancies exhibits enhanced performance in heterogeneous oxidation. In principle, doping 50 mol% divalent cations (such as: Cu2+, Zn2+, and Mg2+) into CeO2 lattice would produce an exceptional catalyst with maximum active oxygen species. However, the huge size gap between Ce (IV) and divalent metal cations obstructs its synthesis. Here, we utilize the theory of increasing configurational entropy with five metal dopants to lower the Gibbs‐free energy, and successfully incorporate 50 mol% divalent metal cations into CeO2 lattice. This unique doping environment endows Ce0.5Zn0.1Co0.1Mg0.1Ni0.1Cu0.1Ox two features: (a) Abundant active oxygen species for excellent performance in volatile organic compounds catalytic oxidation; (b) Bring multi reactive sites, which enable the simultaneous combustion of carbon monoxide, propylene and toluene. Moreover, the increased entropy value makes Ce0.5Zn0.1Co0.1Mg0.1Ni0.1Cu0.1Ox an ultra‐stable catalyst in both thermal and hydrothermal conditions (e.g., Working >200 hr in water‐resistance experiment).

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High-entropy oxide perovskites (HEOPs), the incorporation of five or more elements into ABO 3 , possess great flexibility in the composition and electron structure and thus merit untold scientific and technological potential. However, the conventional synthetic methods at high temperatures tend to obtain the bulk with a low surface area, limited exposed active sites, and result in poor catalytic activity. Herein, we report a metal−tannin coordination assembly strategy to synthesize HEOP nanoparticles (NPs) with a size of 10−30 nm and abundant oxygen vacancies. Interestingly, up to 10 immiscible metal elements could be confined into the single HEOP NPs. Meanwhile, the as-synthesized La(FeCoNiCrMn) 3 NPs exhibit better CO oxidation activity than single-metal−oxide perovskites and the conventionally solidstate prepared HEOP catalysts. Moreover, the entropy-stabilized NPs function well in moistureor SO 2 -containing reaction conditions. This work opens up new opportunities to design nanostructured high-entropy materials for heterogeneous catalysis.