Ultrasonic vibration has been employed to improve the quality of machined surface in the grinding of brittle materials. In this report, we transplant the philosophy of ultrasonic vibration assisted grinding to chemo-mechanical bound-abrasive-pellet polishing in anticipation of the improvement in either surface roughness or material removal rate. The preliminary experimental results show that the ultrasonic vibration assisted chemo-mechanical pellet polishing can yield desired results that material removal rate can be significantly raised while surface roughness is not degraded. The experimental results also indicate different mechanisms between ultrasonic-vibration-assisted chemo-mechanical pellet polishing and conventional chemo-mechanical bound-abrasive polishing.