Exploring electrocatalysts with satisfactory activity and durability has remained a long-lasting target for electrolyzing water, which is particularly significant for sustainable hydrogen fuel production. Here, we report a quaternary B/P-codoped transition metal Co-Mo hybrid as an efficient alternative catalyst for overall water splitting. The Co-Mo-B-P/CF dual nanowafers were deposited on a copper foam by double-pulse electrodeposition, which is favorable for achieving a nanocrystalline structure. The Co-Mo-B-P/CF catalyst shows a high catalytic activity along with good long-term stability in 1.0 M KOH solutions for both the hydrogen and oxygen evolution reactions, requiring 48 and 275 mV to reach 10 mA cm–2, respectively. The synergetic effect between Co-Mo and doped B and P elements is mainly attributed to the excellent bifunctional catalysis performance, while the dual-nanowafer structure endows Co-Mo-B-P with numerous catalytical active sites enhancing the utilization efficiency of atoms. Moreover, the catalytic capability of Co-Mo-B-P/CF as a bifunctional electrocatalyst for the overall water splitting is proved, with the current density of 10 mA cm–2 accomplished at 1.59 V. After the stability test for overall water splitting at 1.59 V for 24 h, the activity almost remains unchanged. The features of excellent electrocatalytic activity, simple preparation, and inexpensive raw materials for Co-Mo-B-P/CF as a bifunctional catalyst hold great potentials for overall water splitting.