We report the successful growth of highly spin-polarized chalcogenide thin films of CuCr{sub 2}Se{sub 4}, which are promising candidates for spin-based electronic applications. We also present electronic structure calculations for CuCr{sub 2}Se{sub 4} that, together with magnetic and transport data, imply that the stoichiometric compound is a metallic ferromagnet with a relatively low density of hole-like carriers at the Fermi energy. These calculations also predict that a deficiency of Se will deplete the minority density of states at the Fermi energy perhaps leading to a half-metal. We have successfully grown thin films of CuCr{sub 2}Se{sub 4} by pulsed laser deposition on isostructural MgAl{sub 2}O{sub 4} substrates followed by an anneal in a Se-rich environment. X-ray diffraction confirms the structure of CuCr{sub 2}Se{sub 4} on MgAl{sub 2}O{sub 4} substrates as well as a secondary phase of Cr{sub 2}Se{sub 3}. X-ray absorption spectroscopy indicates that the chemical structure at the surface of the films is similar to that of bulk CuCr{sub 2}Se{sub 4} single crystals. Magnetization measurements indicate that these films saturate with a magnetic moment close to 5 {micro}{sub B} per formula unit and a T{sub c} above 400 K. X-ray magnetic circular dichroism shows that the magnetism persists to the surface of the film. Resistivity and Hall effect measurements are consistent with a p-type ferromagnetic metallic behavior and with the electronic structure calculations.