We report a novel strategy for the fabrication of mesoporous silica (MS)@CuO@FeS2 composite microsphere-based anisotropic films that combine the advantages of the CuO and FeS2 materials to improve photoelectric conversion. This was achieved by aligning MS@CuO@FeS2 composite microspheres in a cross-linked gel under a homogeneous magnetic field. The MS@CuO@FeS2 composite microspheres, which were synthesized by a simple layer-by-layer (LbL) self-assembly technique together with a solvo-thermal method, can absorb a wide range of light and exhibit ferromagnetic properties. In addition, the resulting MS@CuO@FeS2 composite microsphere-based anisotropic film shows photoelectric anisotropy. Such systems are promising for improving the performance of solar cells. (C) 2013 Elsevier Inc. All rights reserved.