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In this work, we report Co3O4@PPy hybrid structured electrode materials for overall water splitting. The as-synthesized Co3O4/PPy-120 samples present excellent electrocatalytic performances for OER and HER and long durability. It only requires an operating potential of 1.67 V to deliver a current density of 10 mA/cm2 with a remarkable durability for 28 h. The superior electrocatalytic performances mainly can be attributed to the unique heterostructures and the synergistic effects between PPy and Co3O4 electrode materials.