We have studied the effect of chemical-mechanical polishing (CMP) on the ferroelectric, piezoelectric, and microwave dielectric properties of Ba-substituted PZT (BPZT), deposited by pulsed laser deposition. CMP allowed for the reduction of the root mean square surface roughness of 600 nm thick BPZT films from 12.1 ± 0.1 nm to 0.79 ± 0.15 nm. Ammonium peroxide (SC-1) cleaning was effective to remove Si CMP residuals. Measurements of the ferroelectric hysteresis after CMP indicated that the ferroelectric properties of BPZT were only weakly affected by CMP, while the piezoelectric d33 coefficient and the microwave permittivity were reduced slightly by 10%. This can be attributed to the formation of a thin dead layer at the BPZT surface. Moreover, the intrinsic dielectric permittivity at microwave frequencies between 1 and 25 GHz was not influenced by CMP, whereas the dead layer series capacitance decreased by 10%. The results indicate that the CMP process can be used to smoothen the BPZT surface without affecting the film properties strongly.