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This paper reports our recent results on the nanoindentation and nanoscratch of LiTaO3 single crystals. The elastic modulus and hardness of LiTaO3 obtained from nanoindentation were 251±3 GPa and 12.6±0.6 GPa, respectively. During indenting, pop-in events occurred when indentation load was in the range from 305 to 640 μN. Incipient kink bands (IKBs) were believed to be responsible for the pop-ins. Nanoscratching showed that there existed a threshold normal load of 2.5 mN, above which cracks were generated and the material removal was in the brittle regime. The knowledge gained is valuable to the design of an effective machining process for LiTaO3 crystals.