The motion of submerged magnetic microspheres rolling at a glass-water interface has been studied using magnetic rotation and optical tweezers combined with bright-field microscopy particle tracking techniques. Individual microspheres of varying surface roughness were magnetically rotated both in and out of an optical trap to induce rolling, along either plain glass cover slides or glass cover slides functionalized with polyethylene glycol. It has been observed that the manipulated microspheres exhibited nonlinear dynamic rolling-while-slipping motion characterized by two motional regimes: At low rotational frequencies, the speed of microspheres free-rolling along the surface increased proportionately with magnetic rotation rate; however, a further increase in the rotation frequency beyond a certain threshold revealed a sharp transition to a motion in which the microspheres slipped with respect to the external magnetic field resulting in decreased rolling speeds. The effects of surface-microsphere interactions on the position of this threshold frequency are posed and investigated. Similar experiments with microspheres rolling while slipping in an optical trap showed congruent results.