We have prepared entirely (111) oriented C 60 single crystal films on GaAs(100) using the vacuum vapor deposition technique with double temperature zone, and studied the structure and morphology of films using X-ray diffraction and scanning electron microscopy. The results show that the highly oriented growth of C 60 films occurred only at a narrow range of substrate temperature, higher or lower substrate temperature results in random orientation of grains. A preliminary explanation for experimental results is given and the growth mechanism of the C 60 single film is discussed.