In order to achieve an easy fabrication and considerable directional orientation, we use a sedimentation method to prepare composites consisting of FeSiAl flakes. The flakes are dispersed in hydroxylated acrylic resin solution in sonication and natural form into laminated composite samples. Then, the toroidal rings are made with the prepared laminated composite samples. Compared with random orientational FeSiAl flakes in the composite, the complex permeability of laminated sample has been obviously improved when microwave frequency is below 4 GHz, especially for the imaginary part. A model is proposed to explain the formation reason of aligned FeSiAl composite by this method. Damping factor (α) is calculated by the combination of the effective medium theory and Landau-Lifshitz-Gilbert equation, and the permeability of the samples is verified by these theories.