The structural and electronic properties of (CdTe)1−x(In2Te3)x thin films as a function of substrate temperature were studied using x-ray diffraction, energy dispersive x-ray analysis, and Raman, transmission, and modulated transmission spectroscopies. The films were grown by the close-spaced vapor transport technique combined with free evaporation; CdTe and In2Te3 were used as sources. From x-ray diffraction the presence of mixed phases and differences in composition were detected, and good correlation with Raman spectroscopy was found. Transmission spectroscopy suggested the possibility of a modulation of the band gap of the alloy from a value as low as 0.5 eV up to 1.5 eV. Single-phase films presented a direct band gap of around 1.15 eV, as obtained from modulated transmission measurements.