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Thin carbon films have been prepared by ArF excimer laser ablation of hard fullerene-based carbon in vacuum. The target material was obtained from pressure-temperature treatment of C60 fullerene. Micro-Raman, electron energy loss, and electron diffraction measurements of deposited films reveal distinct evidence of a small microcrystalline diamond fraction. This appears to be the observation of crystalline diamond produced by laser ablation of a nondiamond target.