A correlation between orientation evolution and carrier transport 10-nm-thick critical layers (CLs) are made from Ga-doped ZnO films by ion plating. The use of CLs improves grain orientation of Al-doped ZnO films on CLs. The effect of CLs on carrier transport at grain boundaries is demonstrated. 500-nm-thick AZO films with CLs exhibited a high Hall mobility of 50.1 cm2/Vs.