A unique method for nucleating diamond films on surfaces using C clusters is described. The process substitutes the need for diamond polish pretreatment of substrates prior to diamond film growth, as currently practiced in low‐pressure (<1 atm) chemical vapor deposition methods. As an example, the use of C clusters C60 and C70 as nucleating layers on single‐crystal Si surfaces is presented. It is shown that a thin layer (approximately 1000 Å) of pure carbon C70 is sufficient for the nucleation and growth of fine grain polycrystalline diamond films. The enhancement of nucleation by the C70 layer is nearly ten orders of magnitude over an untreated Si surface. It also follows that C clusters can be used as a one‐step lithographic template for growing diamond on selected regions of the substrate. In addition, insight into the mechanism for diamond nucleation from C clusters is given.

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