The efficacy of various non-diamond carbon films as precursors for diamond nucleation on unscratched silicon substrates was investigated with a conventional microwave plasma-enhanced chemical vapor deposition system. Silicon substrates were partially coated with various carbonaceous substances such as clusters consisting of a mixture of C60 and C70, evaporated films of carbon and pure C70, and hard carbon produced by a vacuum are deposition technique. For comparison, diamond nucleation on silicon substrates coated with submicrometer-sized diamond particles and uncoated smooth silicon surfaces was also examined under similar conditions. Except for evaporated carbon films, significantly higher diamond nucleation densities were obtained by subjecting the carbon-coated substrates to a low-temperature high-methane concentration hydrogen plasma treatment prior to diamond nucleation. The highest nucleation density (∼3 × 108 cm−2) was obtained with hard carbon films. Scanning electron microscopy and Raman spectroscopy demonstrated that the diamond nucleation density increased with the film thickness and etching resistance. The higher diamond nucleation density obtained with the vacuum are-deposited carbon films may be attributed to the inherent high etching resistance, presumably resulting from the high content of sp3 atomic bonds. Microscopy observations suggested that diamond nucleation in the presence of non-diamond carbon deposits resulted from carbon layers generated under the pretreatment conditions.