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Chromium-doped hydrogenated diamond-like carbon (Cr-DLC) and chromium carbide hydrogenated DLC alloys were synthesized by plasma-assisted vapor deposition and investigated by x-ray absorption near edge structure spectroscopy, extended x-ray absorption fine structure, and superconducting quantum interference device (SQUID) magnetometry. Structural and magnetic properties of the doped and alloy materials were investigated as a function of the Cr concentration (0.1–20 at. %). Toward the upper end of the concentration range, Cr precipitates in the form of chromium carbide (Cr3C2) nanoclusters. For low Cr concentrations, the systems are ferromagnetic at very low temperatures, whereas the chromium carbide clusters appear to be antiferromagnetic with uncompensated spins at the surface. Cr-DLC films and alloys with various Cr concentrations are used to make heterojunctions on silicon, and the produced diodes are investigated by I-V measurements. The heterojunctions exhibit negative magnetoresistance that saturates at less than 500 Oe and may be suitable for spin-electronics applications.