The morphology of typical CVD diamond thin films has been shown to be controlled by the concentration of methane during deposition. For example, for CH4 concentrations c < 0.4% the (111) faces dominate, while at 0.4% < c < 1.2% (100) faces dominate. Here we showed that the (100) oriented diamond films can be grown on top of the microcrystalline ball-like particles under suitable conditions. These (100) oriented diamond films are grown under the condition of 1.5% methane in hydrogen, substrate temperature of 680 °C–750 °C, and pressure of 30–80 Torr. The bombardment of the diamond thin films by ions in the plasma is believed to be an important factor for the formation of (100) oriented films on top of the ball-like particles. SEM, Raman, and x-ray techniques were used to characterize the deposited (100) oriented diamond thin films.