Stable and efficient photocatalyst is the key important research goals up to now. On account of the dominant performance of Ni2P, g-C3N4 (graphitized carbonitride) and UiO-66 (Universitetet i Oslo) themselves, an orderly-designed assemble of g-C3N4/UiO-66/Ni2P is successfully designed and assembled with capability of high-efficient dye-sensitized photocatalytic H-2 evolution. The electron transport routes are successfully adjusted and the hydrogen evolution is greatly improved. It exhibits synergistic effect on highly efficient photocatalytic hydrogen production. The maximum amount of hydrogen evolution reaches about 200 mu mol for 5 h over the g-C3N4/UiO-66/Ni2P photocatalyst under the 5 W LED white light at 420 nm. The H-2 evolution rate is 12 times high than over g-C3N4. Such synergistically increased effect in photocatalytic properties is certified by related characterization results such as TEM, SEM, XPS, XRD, UV-vis DRS, Transient photocurrent and FT-IR etc. The above studies show that the Ni2P nanoparticles modified on the g-C3N4/UiO-66 provides the more active sites and improves the efficiency of photo generated charge separation. In addition, the possible mechanism of photocatalytic hydrogen production is proposed. (C) 2018 Elsevier Inc. All rights reserved.