The synergistic composite g‐C3N4/Cu3P/UiO‐66 with a uniform three‐dimensional (3D) cubic structure distribution was synthesized by hydrothermal method. The larger spherical particles (UiO‐66) uniformly distributed on the g‐C3N4 flaky nanomaterial and the specific surface area of CNCU‐3 reaches an astonishing 1002.08 (m2/g), which is 23 times than that of the base material g‐C3N4. As a result of that, the addition of CU3P and MOF can effectively improve charge transfer and separation, and improve the hydrogen production activity of photocatalysts. The photocatalytic activity of g‐C3N4/Cu3P/UiO‐66 ternary composite was significantly better than that of monomer g‐C3N4, binary g‐C3N4/Cu3P and g‐C3N4/UiO‐66, especially, the introduction of UiO‐66 significantly increased hydrogen production, and the maximum hydrogen production reach 79 μmol in five hours. Moreover, XRD, SEM, TEM, PL, UV‐vis, XPS prove that Cu3P effectively conduct electrons to promote electron transfer and UiO‐66 provide large specific surface area. The synergistic effect of the these factors plays a key role in photocatalytic activity.