Transistors fabricated from C60 films grown by hot wall epitaxy at higher substrate temperature, showed an order of magnitude increased charge carrier mobility up to 6 cm2 V s. In this letter, the authors present an extensive study of morphology and crystallinity of the fullerene films using atomic force microscopy and grazing-incidence x-ray diffraction. A clear correlation of crystalline quality of the C60 film and charge carrier mobility was found. A higher substrate temperature leads to a single crystal-like faceted fullerene crystals. The high crystalline quality solely brings a drastic improvement in the charge carrier mobility. A gate voltage independent mobility is also observed in these devices which can be attributed to the highly conjugated nature of the C60 thin film.