The planarization of rough polycrystalline diamond films synthesized by DC arc discharge plasma jet CVD was attempted using KrF excimer laser pulses. The effects of laser incidence angle and reaction gases (ozone and oxygen) on etching rate were studied. The temperature change of diamond and graphite with different laser fluences was calculated by computer simulation to explain the etching behavior of diamond films. The calculated threshold energy density for etching of pure crystalline diamond was about 1.7 J/cm2. However, the threshold energy density was affected by the angle of laser incidence. Preferential etching of a particular crystallographic plane was observed through scanning electron microscopy. The etching rate of diamond with ozone was lower than that with oxygen. Also, the etching rate of diamond films at normal laser incidence was lower than that of films tilted at 45° for laser fluences above 2.3 J/cm2. When the angle of incidence was 80° to the diamond surface normal, the peak-to-valley surface roughness was significantly reduced, from 30 μm to 0.5μm.