In this work, the anisotropic Ta2O5 thin films with tilted columnar structures are fabricated using asymmertic bideposition technology. The column angle of the anisotropic Ta2O5 thin film is modulated by controlling the asymmetric deposition angles. It is demonstrated that the asymmetric bideposition can enhance the birefringence of a tilted columnar thin film. It is different from the traditional Tait’s rule that a set of films indicates proportional relationship between the principal indices and the column angle.