Enzymatic sensors have inherent problems such as the low stability and limited pH range in industrial and biomedical applications and therefore, more efficient nonenzymatic sensors are highly desirable. Herein, plasmafunctionalized defective MoSe 2 is prepared and studied as a highly efficient catalyst for electrochemical sensing of H 2 O 2 . Experiments and theoretical computations show that the plasma-induced Se multi-vacancies and nitrogen dopants generate new active sites, expose more edge active surfaces, narrow the bandgap, and strengthen binding with the •OH intermediate, which imparts new fundamental knowledge about the roles of defects in catalysis. The defective MoSe 2 -catalyzed sensor delivers competitive performance in hydrogen peroxide detection such as a low detection limit of 12.6 nmol/L, wide operational pH range of 1−13, good long-term stability, and high selectivity. The portable sensor produced by screen printing confirms the excellent commercial potential and in