Soft magnetic composites (SMCs) have rapidly become the hot spots of research, because of competitive magnetic saturation and high electrical resistivity. Although the magnetic properties have been continuously improved, the nonmagnetic separation and high demagnetization in structure result in low permeability. In this study, Fe-Si-Al SMCs with various particle orientations are designed and prepared under magnetic field. The effects of structures with various orientations on hysteresis loops, effective permeability, magnetic loss and electrical resistance are studied. The results show that the electrical and magnetic properties are totally determined by particle orientation. Especially, compared with non-oriented samples, the permeability of fully oriented samples with particles perpendicular to the normal axis has been greatly improved. This work is of great significance for the research and application of SMCs.