Abstract Simultaneously guaranteeing material removal accuracy and surface quality of robotic grinding is crucial. However, existing studies of robotic grinding process optimization have mainly focused on a single indicator that solely considers contour error or surface roughness, while studies that simultaneously investigate the impact of contact force, spindle speed, feed rate, inclination angle, and path space on the material removal profile (MRP) and the surface roughness are lacking. This paper proposes a hybrid optimization method that considers dimensional accuracy and surface quality constraints. First, an MRP model that considers the coupling influence of the contact force, spindle speed, feed rate, and inclination angle is presented. Then, a surface roughness model that considers the inclination angle is established. Finally, the contact force, feed rate, inclination angle, and path space are simultaneously optimized to satisfy the hybrid constraints of MRP accuracy and surface roughness. The proposed method ensures maximum grinding efficiency while satisfying dimensional accuracy and surface quality constraints. The proposed method is verified on an industrial robotics grinding system with a pneumatic force-controlled actuator. The results show that the proposed method has higher profile accuracy and lower surface roughness than traditional methods.