We demonstrate a critical effect of a metal-to-oxygen ratio on the electrical, optical, and structural properties of ZnO films heavily doped with Ga (carrier concentration in the range of 10(20)-10(21) cm(-3)) grown by plasma-assisted molecular beam epitaxy. The as-grown layers prepared under the metal-rich conditions exhibited resistivities below 3 x 10(-4) Omega cm and an optical transparency exceeding 90% in the visible spectral range as well as a large blue shift of the transmission/absorption edge attributed to the Burstein-Moss shift of the Fermi level deep into the conduction band, indicating high donor concentration. In contrast, the films grown under the oxygen-rich conditions required thermal activation and showed inferior properties. Furthermore, electrical measurements point to the nonuniform depth distribution of free carriers. An oxygen-pressure-dependent surface disordering is suggested to be responsible for the drastic effect of the metal-to-oxygen ratio on the film properties. (C) 2010 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim