Development of a general regulatory strategy for efficient overall water splitting remains a challenging task. Herein, a simple, cost-fairness, and general fluorination strategy is developed to realize surface reconstruction, heteroatom doping, and vacancies engineering over cobalt phosphide (CoP) for acquiring high-performance bifunctional electrocatalysts. Specifically, the surface of CoP nanoarrays (NAs) becomes rougher, meanwhile F doped into CoP lattice and creating amounts of P vacancies by fluorination, which caused the increase of active sites and regulation of charge distribution, resulting the excellent electrocatalyst performance of F-CoP NAs/copper foam (CF). The optimized F-CoP NAs/CF delivers a lower overpotential of only 35 mV at 10 mA·cm⁻² for hydrogen evolution reaction (HER) and 231 mV at 50 mA·cm⁻² for oxygen evolution reaction (OER), and the corresponding overall water splitting requires only 1.48 V cell voltage at 10 mA·cm⁻², which are superior to the most state-of-the-art reported electrocatalysts. This work provides an innovative and feasible strategy to construct efficient electrocatalysts.