The development of an efficient, bifunctional, and affordable catalyst has emerged as a valuable approach for electrocatalysis, as it enhances the charge transfer capability and the number of active sites of the catalyst. Herein, we synthesized a flower-like structure of nickel and iron co-doped molybdenum disulfide on carbon cloth (Ni/Fe-MoS2/CC) using a facile hydrothermal method. The Ni/Fe-MoS2/CC sample exhibited remarkable activity towards the hydrogen evolution reaction, with low overpotentials of −116 mV and a Tafel slope of 43 mV/dec at −10 mA/cm2. It also showed excellent performance in the oxygen evolution reaction with an overpotential of 202 mV and a Tafel slope of 65 mV/dec to afford a current density of + 10 mA/cm2 along with high stability. This study illustrates the beneficial effect of Ni and Fe co-doping on the synthesized flower-shaped MoS2 with the formation of 1 T phase on MoS2/CC, demonstrating significant potential in the field of electrocatalysis.