Molybdenum disulfide (MoS2) is modified by using ambient solution plasma for hydrogen and oxygen evolution reactions (HER and OER). The modified MoS2 exhibits low overpotential of −0.18 V at −10 mAcm−2 for HER and 1.40 V at 10 mAcm−2 for OER with Tafel slope of 95 and 65 mVdec−1, respectively. The improved HER and OER performance is attributed to increased electrochemical active surface area and reduced impedance compared to precursor MoS2. The effect of time dependent plasma treatment on MoS2 is also investigated, indicating that the optimal time (90 min) shows better HER and OER performance.