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To overcome the thermodynamic and kinetic impediments of the Sabatier CO2 methanation reaction, the process must be operated under very high temperature and pressure conditions, to obtain an industrially viable conversion, rate, and selectivity. Herein, we report that these technologically relevant performance metrics have been achieved under much milder conditions using solar rather than thermal energy, where the methanation reaction is enabled by a novel nickel‐boron nitride catalyst. In this regard, an in situ generated HOB⋅⋅⋅B surface frustrated Lewis's pair is considered responsible for the high Sabatier conversion 87.68 %, reaction rate 2.03 mol gNi−1h−1, and near 100 % selectivity, realized under ambient pressure conditions. This discovery bodes well for an opto‐chemical engineering strategy aimed at the development and implementation of a sustainable 'Solar Sabatier' methanation process. [ABSTRACT FROM AUTHOR]