Thin films of pure germanium-carbon alloys (GexC1−x with x ≈ 0.0, 0.2, 0.4, 0.5, 0.6, 0.8, 1.0) have been grown on Si(100) and A12O3 (0001) substrates by pulsed laser ablation in a high vacuum chamber. The films were analyzed by x-ray θ-2θ diffraction (XRD), x-ray photoelectron spectroscopy (XPS), Auger electron spectroscopy (AES), conductivity measurements and optical absorption spectroscopy. The analyses of these new materials showed that films of all compositions were amorphous, free of contamination and uniform in composition. By changing the film composition, the optical band gap of these semiconducting films was varied from 0.00eV to 0.85eV for x = 0.0 to 1.0 respectively. According to the AES results, the carbon atoms in the Ge-C alloy thin film samples has a bonding configuration that is a mixture of sp2 and sp3 hybridizations.