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Reforming methane to produce syngas is a subject that generates considerable interest. The process requires catalysts that possess high-performance active sites to activate stable C–H bonds. Herein, we report a facile synthetic strategy to prepare Ni-based catalysts by complexation–impregnation (Ni-G/SiO₂-C) and precipitation–impregnation (Ni-G/SiO₂-P) methods using glycine as a complexing agent. The particle size of Ni in both types of catalysts is decreased by adding glycine in the preparation process. Nevertheless, the preparation methods and amount of glycine play a significant role in the particle size and distribution of Ni over the Ni-based catalysts. The smaller particle size and narrower distribution of Ni were obtained in the Ni-G/SiO₂-P catalyst. The catalysts were comparatively tested for carbon-dioxide reforming of methane (CDR). Ni-G/SiO₂-P showed better CDR performance than Ni-G/SiO₂-C and Ni/SiO₂ and increased stability because of the smaller particle size and narrower distribution of Ni. Moreover, a high-performance Ni-based catalyst was prepared by optimizing the amount of glycine added. An unobservable deactivation was obtained over Ni-G-2/SiO₂-P and Ni-G-3/SiO₂-P for CDR during TOS = 20 h. Thus, a new promising method is described for the preparation of Ni-based catalysts for CDR.