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The valorization of methane and carbon dioxide is a promising solution for mitigating global warming. The dry reforming of methane (DRM) is capable of concomitant conversion of these greenhouse gases into starting materials for production of synthetic fuels, promoting a carbon-neutral avenue for fuel production. The development of efficient, stable, and economic catalysts presents a challenge owing to the comparatively rapid deactivation of DRM catalysts under reaction conditions. Here, Ni/La2O3DRM catalysts are prepared by combustion synthesis of Ni and La complexes of nitrogen-rich precursors. We expound the relationship between structures of the combustion precursors, the thermochemistry of their combustion, the structures of the resultant Ni/La2O3catalysts, and their performance under DRM conditions. We show that the best catalyst is derived from energetic precursor which have the sharpest exotherm and rapidly releases the largest amounts of nitrogen gas. These properties give rise to the crystallization of Ni/La2O3catalyst with high Ni dispersion and strong metal-support interactions. This work can act as starting point to expand the link between the chemistry of combustion precursors and the resulting catalyst properties, eventually realizing the rational design of high-performance catalysts prepared by combustion synthesis through tailoring the chemistry and structure of the nitrogen-rich precursors.