Anisotropic polyaniline (PAni) plates decorated with self-aligned nanofiber arrays were synthesized under the hydrothermaI conditions. The formation mechanism of the self-assembled structures was investigated by studying the effect on PAni micro-structure with additive electrolyte in reaction system, and numerical simulation for dependence of systematic electrostatic energy on cross angles of self-assembled nanofiber arrays in grid textured PAni plates. It is proposed that the electrostatic interaction based on ionic doping charges plays an important role in the formation of the self-assembled PAni structures.