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Methane reforming with carbon dioxide (DRM) is one promising way to achieve carbon neutrality and convert methane to syngas for high-value chemical production. Catalyst development with better performance is the key to its potential large-scale industrial application due to its deactivation caused by carbon deposition and metal sintering. Hence, a Ni/CeO₂ catalyst (Ni/CeO₂-M) with higher CO₂ conversion and better stability is prepared, supported on CeO₂ precipitated via a novel microimpinging stream reactor. A series of ex-situ or in-situ characterizations, such as CO titration measurements, two-step transient surface reaction (two-step TSR), CO₂ and CH₄ temperature-programmed surface reaction (CO₂-TPSR and CH₄-TPSR), X-ray absorption fine structure (XAFS), and in-situ Raman spectroscopy study, were used to investigate its structure and mechanism. In contrast to Ni supported on commercial CeO₂ (Ni/CeO₂-C), the Ni/CeO₂-M catalyst with stronger lattice oxygen mobility and higher oxygen storage capacity enhances its CO₂ activation ability and carbon deposition. The Ni particle size of the Ni/CeO₂-M catalyst decreased, and a higher oxidation state was obtained due to the strong metal–support interaction. Besides the reaction performance improvement of the Ni/CeO₂-M catalyst, the novel microimpinging stream reactor could achieve catalyst continuous production with a high preparation efficiency. This work provides a novel method for the high-performance catalyst preparation for DRM reaction and its mechanism study gives a deep insight into high-performance catalyst development via bottom-up study.