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A catalytically assisted etching method, named Catalyst-Referred Etching (CARE) was applied to the planarization of Lithium Niobate (LN) surface, which is widely used for optical waveguides, optical modulators, piezoelectric applications. The study demonstrates that an atomically smooth surface with less than 0.1 nm root-mean-square roughness could be achieved on a LN substrate using a thin metal film and pure water as the catalyst and etching solution, respectively. All residual stress and surface damage could be removed completely thanks to the removal mechanism of CARE.