The electrochemical nitrate reduction reaction (NO 3− RR) has an important application value in realizing efficient synthesis of ammonia (NH 3 ) from NO 3 − , and obtaining a highperformance and low-cost electrocatalyst is the key. Nonetheless, a majority of the existing catalysts for the NO 3 − RR have the problem of an unsatisfactory NH 3 yield and insufficient stability. Herein, a heterostructured CoS 2 /MoS 2 electrocatalyst is designed and fabricated, and the structure−activity relationship is studied. In comparison to pure CoS 2 and MoS 2 , CoS 2 /MoS 2 demonstrates an enhanced performance with 2.8 and 2.0 times the current enhancement, respectively, at an applied potential of −0.25 V versus reversible hydrogen electrode. It is found that the electronic structure of CoS 2 /MoS 2 is modified through electron transfer between Co and Mo for enhanced reaction dynamics. Moreover, in heterostructured CoS 2 /MoS 2 , the two components (CoS 2 and MoS 2 ) cooperate well with each other to tailor reaction steps of the NO 3 − RR. Eventually, CoS 2 /MoS 2 achieves a faradaic efficiency of 97.07%, NH 3 yield rate of 0.44 mmol h −1 cm −2 , NO 3 − conversion rate of 75.43%, and NH 3 selectivity of 95.45% in a 1.0 M KOH electrolyte with 600 ppm of NO 3 − -N, retaining its promising applications in the NO 3 − RR.