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Controlling the selectivity of CO 2 hydrogenation by catalysis is a fundamental challenge. This study examines the interrelation between active sites and reaction pathways in Ni-catalyzed CO 2 hydrogenation. The alloying of Ni with Zn to charged (Ni σ− −Zn σ+ ) active sites modifies the electronic structure and d-band center, weakens the interaction with CO/H 2 , and preferentially catalyzes the reverse water gas shift to CO with the thermodynamically favored methanation pathway switched off. The charged dual sites can stabilize the activated CO 2 species in a η 2 (C, O) bridge configuration, directly dissociate the CO bond to *CO, and promote CO desorption. The mechanistic investigation has elucidated the reaction pathways in the Ni-catalyzed CO 2 hydrogenation and identified the crucial intermediates that impacted the product selectivity, which can provide a theoretical guide for the Ni-based catalyst design.

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