Al-doped zinc oxide (AZO) films were deposited by means of remote plasma-enhanced metalorganic chemical vapor deposition from oxygen/diethylzinc/trimethylaluminum mixtures. The electrical, structural (crystallinity and morphology), and chemical properties of the deposited films were investigated using Hall, four point probe, x-ray diffraction (XRD), scanning electron microscopy (SEM), atomic force microscopy (AFM), electron recoil detection (ERD), Rutherford backscattering (RBS), and time of flight secondary ion mass spectrometry (TOF-SIMS), respectively. We found that the working pressure plays an important role in controlling the sheet resistance Rs and roughness development during film growth. At 1.5 mbar the AZO films are highly conductive (Rs4% of the film thickness), however, they are characterized by a large sheet resistance gradient with increasing film thickness. By decreasing the pressure from 1.5 to 0.38 mbar, the gradient is significantly reduced and the films become smoother, but the sheet resistance increases (Rs100 / for a film thickness of 1000 nm). The sheet resistance gradient and the surface roughness development correlate with the grain size evolution, as determined from the AFM and SEM analyses, indicating the transition from pyramid-like at 1.5 mbar to pillar-like growth mode at 0.38 mbar. The change in plasma chemistry/growth precursors caused by the variation in pressure leads to different concentration and activation efficiency of Al dopant in the zinc oxide films. On the basis of the experimental evidence, a valid route for further improving the conductivity of the AZO film is found, i.e., increasing the grain size at the initial stage of film growth.