Fine powders composed of tellurium grains of average size <10 nm were produced by dry vibration milling combined with liquid-phase sedimentation techniques, starting from polycrystalline powders with average grain diameter of ca. 30 μm. Nanocomposite films were obtained by binding the nanosized tellurium grains with poly(methyl methacrylate). Raman spectroscopy revealed that the films were based on the coexistence of tellurium and tellurium oxide crystalline phases due to a partial oxidation in air of the grains. The optical measurements of the fabricated material showed that the absorbance was nearly constant in the 310–2200 nm range and that a typical UV absorption peak of the nanostructured tellurium was centered at around 260 nm. An extensive characterization of the photoconductivity properties was carried out by illuminating the tellurium-poly(methyl methacrylate) films with white light or radiations of different spectral composition selected from the UV–Vis-NIR region. Data analysis has allowed to demonstrate that the photoresponse is closely related to the optical absorption and is independent of the spectral composition of the incident radiation in the wavelength range from 310 to 2200 nm, while the photocurrent increases linearly as a function of the optical power density over about three orders of magnitude.