We have investigated polarized Raman spectra of (001)/(100)-oriented tetragonal epitaxial Pb(ZrxTi1-x)O3 (PZT) thin films (x=∼0.35) in which the volume fraction of the polar c domain is systematically varied from 4% to 96%. From polarization analyses using high epitaxial quality films, we have successfully isolated the A1 and B1 phonons from the E phonons, thus offering a distinctive evaluation of the c domains. As increasing c-domain volume, the A1(TO) modes linearly increase in their intensity. A remarkable correlation is found between the A1(1TO)-mode intensity and the c-domain volume for PZT films. We suggest that this correlation as well as the A1(1TO)-mode intensity provide a simple and useful probe for characterization of c-domain volume and ferroelectric properties in PZT-based devices.