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Developing cost‐effective, high‐performance nitrogen reduction reaction (NRR) electrocatalysts is required for the production of green and low‐cost ammonia under ambient conditions. Here, a strategy is proposed to adjust the reaction preference of noble metals by tuning the size and local chemical environment of the active sites. This proof‐of‐concept model is realized by single ruthenium atoms distributed in a matrix of graphitic carbon nitride (Ru SAs/g‐C₃N₄). This model is compared, in terms of the NRR activity, to bulk Ru. The as‐synthesized Ru SAs/g‐C₃N₄ exhibits excellent catalytic activity and selectivity with an NH₃ yield rate of 23.0 µg mg_cat⁻¹ h⁻¹ and a Faradaic efficiency as high as 8.3% at a low overpotential (0.05 V vs the reversible hydrogen electrode), which is far better than that of the bulk Ru counterpart. Moreover, the Ru SAs/g‐C₃N₄ displays a high stability during five recycling tests and a 12 h …