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The electrochemical nitrogen reduction reaction (NRR) is an attractive process for next‐generation ammonia synthesis; therefore, identifying a suitable catalyst for this reaction is critical. In recent years, transition‐metal dichalcogenides (TMDs) and their Janus structures have gained significant attention because of their outstanding catalytic properties. However, the synthesis of Janus TMDs remains challenging, and exposing their active sites is difficult when using a low‐dimensional structure to improve the catalytic activity. To date, relatively little research has been conducted in this area. Herein, emerging Janus WSeS/WSe2 heterostructure nanowalls are systematically explored. These nanowalls are used as a nitrogen fixation catalyst in electrolytes. The nanowalls demonstrate a significant NH3 yield rate and Faradaic efficiency of 13.97 µg h‐mgcat−1 and 35.24% at −0.3 V in 0.1 m HCl, as well as 15.96 µg h‐mgcat−1 and 40.2% in 0.1 M Na2SO4. This study presents an in‐depth analysis of the properties of Janus WSeS/WSe2 heterostructure nanowalls and a conceptual framework for linking TMD‐based catalysts and the NRR. [ABSTRACT FROM AUTHOR]