Epitaxial films of (1−x)Pb(Yb1/2Nb1/2)O3−xPbTiO3 (PYbN–PT, x=0.4,0.5) with SrRuO3 bottom electrodes were prepared on (100) LaAlO3, (100) SrTiO3, and (111) SrTiO3 substrates by pulsed laser deposition. It was found that vacuum annealing of the SrRuO3 before the deposition of PYbN–PT facilitated growth of perovskite PYbN–PT. With optimized growth conditions, (001) and (111) PYbN–PT epitaxial films with good phase purity were obtained in a range of 650–660 and 600–620 °C, respectively. The ferroelectric and transverse piezoelectric properties of these PYbN–PT films were investigated. In the (001) PYbN–PT (50/50) film, the highest remanent polarization (∼30 μC/cm2) and e31,f piezoelectric coefficient (−14 C/m2) were observed. The transition temperature of the (001) PYbN–PT (50/50) film was near 380 °C.