To improve the growth rate of chemical vapor deposition (CVD) diamond coating, increasing the chemical reaction rate is essential. A novel method of dispersing graphene oxide (GO) particles as adsorbent on the substrate prior to deposition was proposed, with which the diamond coating with large grain size and high thickness was deposited on the silicon nitride under the normal CVD environment. The as-deposited diamond coating was characterized by scanning electron microscopy (SEM), surface profilometer, atomic force microscope (AFM), Raman spectrum, and indentation. The surface morphologies showed that the GO particles were covered by a layer of diamond coating. The diamond coating without and with GO particles had growth rates of 1.10–1.38 and 1.50–2.94 μm h−1, respectively. No differences in the Raman spectra of the microcrystalline diamond (MCD) coatings without and with GO particles were found. Indentation tests suggested that GO particles could enhance the adhesive strength and the crack resistance of diamond coating, which may result from the large thickness and the strong adsorbed capacity of destructive energy. Hence, dispersing particles on the substrate can be regarded as a potential and alternative technique by accelerating the CVD chemical reaction to obtain desired diamond coating.