Cesium Lithium Borate (CsLiB6O10 or CLBO) is the most effective non-linear crystal which generates ultraviolet harmonics of the Nd:YAG fundamental laser wavelength. In order to enhance the damage threshold, low CLBO surface roughness, by ultra-precision machining, is needed. Because the CLBO crystal has easy hydroscopic reaction and micro scratches in machining, ultra-precise machining of the CLBO crystal is a difficult technical problem. In this paper, the new lapping slurry and polishing slurry are introduced. And the deliquescence degree of CLBO is fallen to lowest. A new working technology is also adopted. After rough polishing, the concentration of ultra-precision polishing slurry is increased properly. So does the ultra-precision polishing speed, and the wiping speed is faster than the deliquescence speed. The CLBO crystal surface roughness can achieve 1nm and keep the surface quality well.