We report the fabrication of crystalline microresonators of high quality (Q) factors with a controllable wedge angle on lithium niobate on insulator (LNOI). Our technique relies on a femtosecond laser assisted chemo-mechanical polish, which allows us to achieve ultrahigh surface smoothness as critically demanded by high Q microresonator applications. We show that by refining the polish parameters, Q factors as high as 4.7 × 107 can be obtained and the wedge angle of the LNOI can be continuously tuned from 9° to 51°.