To improve the electrolysis efficiency of overall water splitting, designing an efficient and stable catalyst becomes very essential. Herein, a one-step cyclic voltammetric electrodeposition method was adopted to synthesize a low-crystallinity NiFeCoPi/P catalyst by adding Fe and Co to NiPi/P. The synthesized NiFeCoPi/P catalyst exhibits good catalytic performance for hydrogen evolution reaction (HER) in 1 M NaOH and oxygen evolution reaction (OER) in 0.5 M Na2CO3/NaHCO3, showing low overpotentials of 98 and 299 mV for HER and OER at 10 mA cm(-2), respectively. Also, the electrodeposition only requires a cell voltage of 1.63 V for overall water splitting. It could be found that the introduction of Fe and Co can enhance charge transport among the metals and can effectively change the morphology of the catalyst, thus increasing the electrocatalytic performance for HER and OER. Moreover, the NiFeCoPi/P catalyst reveals good stability in the electrolysis process of overall water splitting.