The effects of the isoelectronic Al doping of epitaxial GaN films grown by metalorganic chemical vapor deposition on a (0001) Al2O3 single crystal substrate were investigated. It was found that the threading screw and edge dislocation densities of the GaN film decreased to less than half of that of the undoped GaN film up to Al doping concentration of 0.45%. The in-plane and out-of-plane strains were simultaneously reduced with the decrease in dislocation density as a result of the solution hardening effect. Accordingly, the electron mobility of the 0.45% Al-doped GaN film (524 cm2/Vs) was greatly improved compared to that of the undoped GaN film (178 cm2/Vs). However, the threading dislocation densities and strains were increased at a 0.64% Al concentration, and the electron mobility decreased accordingly. Therefore, the improvement in the electron mobility by Al doping up to 0.45% is the result of a decrease in the threading dislocation density and not a decrease in the number of point defects (Ga-site vacancy) as suggested earlier [Lee et al., Appl. Phys. Lett. 83, 917 (2003)]. © 2004 American Institute of Physics.