Epitaxial CuInSe2 and Cu1In3Se5 films have been synthesized on GaAs(001) by cosputtering Cu∕In and evaporating Se method. Scanning electron micrograph results show that surface morphologies of CuInSe2 and Cu1In3Se5 epitaxial films are substantially different. The rectangular pits of CuInSe2 films imply that the surface energy of (112)B[Se-terminated] is lower than (112)A[metal-terminated] in chalcopyrite CuInSe2 crystals. Nevertheless, the square pits of the Cu1In3Se5 films lead to the conclusion that (112)A and (112)B have almost the same surface energies in the defect-ordered chalcopyrite Cu1In3Se5 crystals. It implies that charge compensation between (112)A and (112)B facets is the driving force of the square pits formation in Cu1In3Se5 crystals.