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Electrochemical nitrogen reduction reaction(eNRR)is an alternative promising manner for sustainable N2 fixation with low-emission.The major challenge for developing an efficient electrocatalyst is the cleaving of the stable N≡N triple bonds.Herein,we design a new MoS2 with in-plane defect cluster through a bottom-up approach for the first time,where the defect cluster is composed of three adjacent S vacancies.The well-defined in-plane defect clusters could contribute to the strong chemical adsorption and activation towards inert nitrogen,achieving an excellent eNRR performance with an ammonia yield rate of 43.4±3 μg h-1 mgcat-1 and a Faradaic efficiency of 16.8±2％at-0.3 V(vs.RHE).The performance is much higher than that of MOS2 with the edge defect.Isotopic labeling confirms that N atoms of pro-duced NH4+originate from N2.Furthermore,the in-plane defect clusters realized the alternate hydrogena-tion of nitrogen in a side-on way to synthesize ammonia.This work provides a prospecting strategy for fine-tuning in-plane defects in a catalyst,and also promotes the progress of eNRR.