A deterministic figuring method for cylindrical surface based on abrasive belt polishing is proposed in this study in order to improve the geometric accuracy of metal shaft parts. The principal motion of material removal is performed through the axial oscillation of the abrasive belt, and the different material removal at different positions can be obtained through servo control of the machine tool spindle by removing high error spots on the cylindrical surface and finally deterministically corrects the roundness error. An abrasive belt-based deterministic figuring device was built, and the figuring experiments were performed on the surface of steel workpieces 100 mm in diameter and 130 mm in effective length. The roundness errors of the entire workpiece after twice figuring iterations decreased nearly from the initial 3 μm to 1 μm, which preliminary verified the feasibility of this method. This deterministic figuring method is expected to break the machining accuracy limit and improve the rotation precision of the precision shaft parts such as the aerostatic spindle.