The optical properties of quaternary AlxInyGa1−x−yN alloy films with 0.16<x<0.64 and 0.02<y<0.13 are presented. The (0001)-oriented AlInGaN layers were grown by metal-organic vapor phase epitaxy on thick GaN/sapphire templates. High-resolution x-ray diffraction measurements revealed the pseudomorphic growth of the AlInGaN films on the GaN buffer. Rutherford backscattering and wavelength-dispersive x-ray spectroscopy analysis were used in order to determine the composition of the alloys. The ordinary dielectric function (DF) of the AlInGaN samples was determined in the range of 1–10 eV by spectroscopic ellipsometry (SE) at room temperature (synchrotron radiation: BESSY II). The sharp onset of the imaginary part of the DF defines the direct absorption edge of the alloys. At higher photon energies, pronounced peaks are observed in the DF indicating a promising optical quality of the material. These features are correlated to the critical points of the band structure (van Hove singularities). An analytical model, which permits us to accurately describe the dielectric function (or optical constants) in the range of 1–10 eV, is also presented. The band-gap and high-energy interband transition values are obtained by fitting the experimental DF with the analytical model. The strain influence on the bandgap is evaluated by using the k×p formalism. Furthermore, an empirical expression is proposed which allows us to calculate the AlInGaN band-gap and high-energy inter-band transitions in the whole compositional range (x, y). The band-gap values obtained from the empirical expression are in good agreement with both the calculated ab initio and the experimental values determined by SE.