Entirely (111) oriented C60 single films are grown successfully on GaAs (100) substrate by a physical vapor deposition technique with double temperature zone.The structure and morphology of films are studied by X-ray diffraction and SEM.The results show that the highly oriented growth of C60 films occurs only at narrow range of substrate temperature,higher or lower substrate temperature leads to random orientation of grains.A reasonable explanation for experimental results is given and the growth mechanism of C60 epitaxial films is discussed.