Synthesis of highly efficient and robust catalysts with earth-abundant resources for overall water splitting is essential for large-scale energy conversion processes. Herein, a series of highly active and inexpensive Co-Ni-P films were fabricated by a one-step constant current density electrodeposition method. These films were demonstrated to be efficient bifunctional catalysts for both H and O evolution reactions (HER and OER), while deposition time was deemed to be the crucial factor governing electrochemical performance. At the optimal deposition time, the obtained Co-Ni-P-2 catalyst performed remarkably for both HER and OER in alkaline media. In particular, it requires -103 mV overpotential for HER and 340 mV for OER to achieve the current density of 10 mA cm, with corresponding Tafel slopes of 33 and 67 mV dec. Moreover, it outperforms the Pt/C//RuO catalyst and only needs -160 mV (430 mV) overpotential for HER (OER) to achieve 200 mA cm current density. Co-Ni-P electrodes were also conducted for the proof-of-concept exercise, which were proved to be flexible, stable, and efficient, further opening a new avenue for rapid synthesis of efficient, flexible catalysts for renewable energy resources.