A 30 kW-powered DC Arcjet Plasma enhanced chemical-vapor deposition (CVD) system was applied to grow diamonds which included the nano-crystal free-standing film, the nano-/micro-crystal layered free-standing film, the gradient micro-crystal free-standing film and the millimeter-sized grain. The free-standing film quality, such as the roughness, the sp 2 content, the residual stress and the grain morphology, was studied by an atomic force microscope (AFM), Raman spectra, a scanning electron microscope (SEM) and a high resolution electron microscope (HREM). In large-sized grain deposition, as-grown deposit was obtained about 1 × 1 × 1 mm 3 in size under the condition of 10 μm/h of the substrate moving speed without Nitrogen enhancement. Characterized by Raman spectra and Laue back reflection X-ray diffraction, the deposit was proven to be single crystal diamond with small grains coving its surfaces. The growth rate was about 30 μm/h. Optical emission spectrum (OES) was utilized to characterize gas phases in the plasma for diamond deposition. The mean electron temperature (Te) in the plasma was calculated based on the value of the emission intensity ratio of I H γ / I H β . Te varied from 0.33 eV to 0.5 eV depending on the concentration of CH 4 in H 2 from 1.0% to 25%. C 2 radical was found to be the dominant carbon source compared with CH radical. The influence of the radical on the morphology of diamond was discussed. It was found that the nano-crystal could be grown when the ratio of the emission intensity, I C 2 / I CH, was larger than 8.