We grew the epitaxial Pb(Zr1-xTix)O3 [PZT] and (1-x)Pb(Mg1/3Nb2/3)O3-xPbTiO3 [PMN-PT] films, above 2 μm in thickness, on (100)cSrRuO3//(100)SrTiO3 substrates by metalorganic chemical vapor deposition (MOCVD). PbTiO3 content (x) dependencies of the crystal structure, dielectric and piezoelectric properties were systematically investigated for these films. The constituent phase changed from a rhombohedral (pseudocubic) single phase, a mixture phase of rhombohedral (pseudocubic) and tetragonal phases, and a tetragonal single phase with increasing x for both of PZT and PMN-PT films. The mixture phase region was observed when x=0.40−0.60 for PZT films and x=0.40−0.55 for PMN-PT films, which became wider than that reported ones for PZT sintered bodies and PMN-PT single crystals. In addition, x value moves to the higher one than that reported for the single crystal and/or the sintered body in case of PMN-PT films, while was almost the same in case of PZT films. The dependence of relative dielectric constant εr was maximum at the mixed phase region for both films, which were similar to the case of their bulk materials. The higher value of εr was ascertained for the PMN-PT films compared with PZT films, however, the magnitude was lower than the reported one for bulk materials. The longitudinal electric-field-induced strain Δx33 and transverse piezoelectric coefficient e31,f for PZT films were also maximum at the mixed phase region, on the other hand, that for PMN-PT films were maximum at larger x edge of rhombohedral (pseudocubic) region. Almost the same order of Δx33 was observed under applied electric fields up to 100 kV/cm, while larger e31,f was observed in PMN-PT films compared with the case of PZT films. e31,f coefficients of ∼−8.9 C/m2 and ∼−11.0 C/m2 were calculated for the PZT film with x=0.46 and for the PMN-PT film with x=0.39, respectively.