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A successful experimental synthesis of pure crystalline β-and α-C3N4 films on Si( 100) substrate was carried out by bias-assisted hot filament chemical vapor deposition (bias-HFCVD). It is found that a mixed-phase C3-x-Six-Ny buffer layer was formed between the Si substrate and the C-N film. A “lattice match selection” was proposed to study the growth mechanism of C3N4 clusters composed of many crystal columns with hexagonal facets.