Development of efficient, low cost, and durable electrocatalysts for oxygen evolution is considered as the key challenge to realize large-scale water splitting. In this work, a novel approach for the synthesis of self-supported carbon coated molybdenum oxide catalyst is reported. An in-situ polymerization strategy is introduced to construct the conductive polypyrrole (PPy) growing on carbon cloth (CC). Subsequently, Mo-O nanoparticles are formed and embedded into the carbon scaffold to form the self-supported oxygen evolution reaction (OER) catalyst on CC with no binders. Further, introducing the metal Ni led to a positive synergistic effect and the Mo-Ni-based bimetallic oxide exhibited an extremely low overpotential of similar to 320 mV to reach a current density of 10 mA cm(-2), which is much lower than the values of most reported transition-metal-based electrocatalysts for OER. Such excellent OER activity is attributed to the well-dispersed and abundant Mo-Ni-O nanoparticles (NPs) on CC and synergistic contribution of Mo-Ni electron density redistribution and excellent electron transfer efficiency between active species and substrate.