Lithium tantalate (LiTaO3) has piezoelectric, electro-optical and nonlinear optical characteristics, and a wide transparency range going from ultraviolet to infrared. It is desirable that LiTaO3 wafer was a smooth surface in order to function with good quality. Chemical mechanical polishing (CMP) has been used to planarize integrated circuits (ICs) or obtain a high surface quality of the substrates. This paper investigates the effect of citric acid as an additive in the slurry for LiTaO3 CMP. The roughness of the wafers was measured by an atomic force microscopy (AFM, XE-100) after polishing. The slurry, which contains citric acid as an additive, has a higher material removal rate and friction force than a slurry without an additive. After polishing, the surface roughness of the LiTaO3 wafer can be reduced down to 1.7Å of Ra.