Aerogel nanoparticles prepared with various Al concentrations were used as a target for the deposition of (V,Al) co-doped ZnO films by rf-magnetron sputtering on glass substrates. The influence of Al content on the structural and the optical properties of the Zn(V,Al)O films was investigated by X-ray diffraction and spectroscopic ellipsometry (SE). It is found that all films exhibit one high intensity (0 0 2) peak, indicating that they have c-axis preferred orientation due to self-texturing mechanism. SE measurements, used to determine the complex pseudo dielectric functions, were carried out at room temperature in the 1–6 eV photon energy region. The excitonic edge of the fundamental band gap (E0) transition in the imaginary part of the dielectric function of the Zn(V,Al)O films is observed around 3.5 eV and shows a dependence on the Al content. The E0 absorption edge of the Zn0.9−x V0.1AlxO alloys shows a blueshift from that of pure ZnO, reaching 389 meV for x = 0.02. This blueshift is interpreted by the Burstein-Moss effect. By analyzing the dielectric function, reduced effective mass m* of the Zn0.9−x V0.1AlxO alloy is extracted and shows good agreement with literature values.