In this study, cobalt phosphide (CoP2) was synthesized onto a Nickel foam (NF) support via phosphorylation under an N2 atmosphere. The resulting material was then coated with tetrahydroxyquinone (THQ), a conjugated microporous polymer, using a hydrothermal method. The as-synthesized CoP2/THQ@NF showed remarkable electrocatalytic performance for the hydrogen evolution reaction and excellent durability in acidic electrolytes. This was attributed to the synergistic effect of the NF support, CoP2, and THQ, which led to a modified electronic structure of CoP2 and a high electron transfer rate of THQ. A low overpotential of 137 mV was required in a 0.5 M H2SO4 solution to achieve a current density of 10 mA cm−2.