2 inch-diameter GaN films with homogeneous thickness distribution have been grown on AlN/Si(111) hetero-structures by pulsed laser deposition (PLD) with laser rastering technique. The surface morphology, crystalline quality, and interfacial property of as-grown GaN films are characterized in detail. By optimizing the laser rastering program, the ~300 nm-thick GaN films grown at 750 °C show a root-mean-square (RMS) thickness inhomogeneity of 3.0%, very smooth surface with a RMS surface roughness of 3.0 nm, full-width at half-maximums (FWHMs) for GaN(0002) and GaN(102) X-ray rocking curves of 0.7° and 0.8°, respectively, and sharp and abrupt AlN/GaN hetero-interfaces. With the increase in the growth temperature from 550 to 850 °C, the surface morphology, crystalline quality, and interfacial property of as-grown ~300 nm-thick GaN films are gradually improved at first and then decreased. Based on the characterizations, the corresponding growth mechanisms of GaN films grown on AlN/Si hetero-structures by PLD with various growth temperatures are hence proposed. This work would be beneficial to understanding the further insight of the GaN films grown on Si(111) substrates by PLD for the application of GaN-based devices.