In this paper, we for the first time report the catalytic activity and durability of nickel cobaltite telluride (NiCo2Te4) nanocluster bifunctional catalysts can be significantly boosted by surface modification with perylenetetracarboxylic-dianhydride for overall water-splitting in neutral solution. We reveal that tuning energy distribution of nanoclusters via a simple surface ligand can drastically increase the catalytic activity towards efficient hydrogen and oxygen evolution reaction simultaneously. A two-electrode based water electrolysis cell using this newly developed nanocluster catalyst operates at a low bias voltage of 1.55 V to achieve a current density of 10 mA.cm(-2) in near-neutral pH solution for overall water-splitting. This, to the best of our knowledge, represents the most efficient mixed-transition-metal-based electrode that has so far been reported for electrochemical water splitting.