Abstract Among high-k thin films, perovskite BaTiO3 (BTO) is an attractive candidate due to its exceptionally high dielectric constant. In contrast to conventional atomic layer deposition (ALD), plasma-enhanced ALD (PEALD) has several advantages such as lower process temperature, improved film quality and the deposition of a wider spectrum of materials. We report the successful deposition of high-k BTO thin films by PEALD. Compositional, morphological, and crystallographic characterizations of PEALD BTO are presented. The electrical performance of PEALD BTO thin films as a function of Ba-to-Ti-ratio is shown. Slightly Ti-rich BTO has the lowest equivalent oxide thickness while Ba-rich films show the lowest leakage current.