A novel and highly efficient three-component Au@CdS/MIL-101 heterostructure was successfully synthesized. The MIL-101(Cr) with large surface area was introduced as a matrix for the well-dispersed growth of Au nanoparticles, and the CdS was selectively coated on the Au nanoparticles. Under visible light irradiation, the Au@CdS/MIL-101 heterostructure presents superior hydrogen evolution rate over the pure CdS, CdS/MIL-101 and Au/MIL-101 composites. The Au@CdS/MIL-101 heterostructure exhibits an unusual H-2 production rate of 250 mu mol h(-1)/10 mg, which is 2.6 times higher than that of pure CdS. The performance enhancement of Au@CdS/MIL-101 heterostructure can be attributed to the following reasons: (i) the large surface area of MIL-101(Cr) can effectively disperse the Au and CdS nanoparticles, resulting in more active adsorption sites and reaction centers. (ii) the strong surface plasmon resonance absorption of Au could accelerate the charge transfer and extend the light response spectrum of CdS. This three-component Au@CdS/MIL-101 heterostructure combining the large surface area of MOF and the surface plasmon resonance of Au into a single structure may provide a potential way to design highly efficient and solar-energy-harvesting photocatalysts. (C) 2015 Elsevier B.V. All rights reserved.