Heteroatom doping is one of the effective ways to improve the catalytic performances of nanozymes. In the present work, the plasma-assisted controllable doping of nitrogen (N) into MoS 2 nanosheets has been initially proposed, resulting in efficient nanozymes. The so-obtained nanozymes were characterized separately by TEM, XRD, XPS, and FTIR. It was discovered that the resulting N-doped MoS 2 nanosheets could present dramatically enhanced peroxidase-like catalytic activities depending on the plasma treatment time. Particularly, that with the 2-min treatment could display the highest catalytic activity, which is over 3-fold higher than that of pristine MoS 2 , that was also demonstrated by the kinetics studies. Herein, the N 2 plasma treatment could facilitate the N elements to be doped covalently into MoS 2 nanosheets to achieve the increased surface wettability and affinity of nanozymes for the improved access of the electrons and substrates of catalytic reactions. More importantly, the covalent doping of N elements into MoS 2 nanosheets with a lower Fermi level, as evidenced by the DFT analysis, could facilitate the promoted electron transferring, resulting in the enhanced catalysis of N-doped MoS 2 nanozymes, in addition to the high catalytic stability in water. Such a controllable plasma treatment strategy may open a new door toward the large-scale applications for doping heteroatoms into various nanozymes with improved catalysis performances.