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Photocatalytic nitrogen (N2) fixation suffers from low efficiency due to the difficult activation of the strongly nonpolar NN bond. In this study, a Ru–Co bimetal center is constructed at the interface of Ru/CoSx with S‐vacancy on graphitic carbon nitride nanosheets (Ru‐Vs‐CoS/CN). Upon adsorption, the two N atoms in N2 are bridged to the Ru–Co center, and the asymmetrical electron donation from Ru and Co atoms to N2 adsorbate highly polarized NN bond to double bond order. The plasmonic electric‐field‐enhancement effect enables the Ru/CoSx interface to boost the generation of energetic electrons. The Schottky barrier between Ru and CoSx endows the interface with electron transfer from CoSx to Ru. The Ru‐end bound N at the Ru–Co center is preferentially hydrogenated. As a result, the Ru‐Vs‐CoS/CN photocatalyst shows an NH3 production rate of up to 0.438 mmol g−1 h−1, reaching a high apparent quantum efficiency of 1.28% at 400 nm and solar‐to‐ammonia efficiency of 0.042% in pure water under AM1.5G light irradiation.

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