Pneumatic polishing tools are commonly used in traditional robot mold polishing systems, but they have problems with the stable control of mold surface roughness due to low precision and poor adaptability in polishing force adjustment. The integration of an adaptive hydraulic polishing (AHP) tool and robot system effectively solves the above problems, providing a robust solution for the high-precision polishing of various molds. This study systematically investigates the robotic polishing of NAK80 mold steel using an AHP-equipped robotic platform with 3M abrasive discs of progressively refined grit sizes (P180, P400, P800). Through single-factor experiments and response surface methodology, the effects of polishing force, rotational speed, and feeding speed on surface roughness were quantitatively analyzed. The relationship between surface roughness and the polishing parameters was derived to elucidate the roughness evolution before and after over-polishing. Orthogonal experiments combined with range analysis identified optimal parameter combinations for P180 (20 N polishing force, 5000 RPM rotational speed, and 5 mm·s⁻¹ feeding speed) and P400 abrasives (10 N polishing force, 4000 RPM rotational speed, and 5 mm·s⁻¹ feeding speed), achieving minimum surface roughness values of 0.08 µm and 0.044 µm, respectively. For P800 abrasives, a central composite design was used to develop a roughness prediction model with a ≤7.14% relative error, and the optimal parameters are a 20 N polishing force, a 5000 RPM rotational speed, and a 5 mm·s⁻¹ feeding speed. The sequential application of the optimized parameters across all the grit sizes can reduce the surface roughness from an initial 0.4 µm to a final 0.017 µm, representing a 95.75% improvement in the surface finish.