High quality BaTiO3 epitaxial thin films on MgO substrates have been grown by pulsed laser deposition (PLD). Both c-axis and a-axis orientated BaTiO3 were studied. Mach-Zehnder (M-Z) optical waveguide modulators have been fabricated by ion beam etching. The BaTiO3 waveguide propagation losses are 1-2 dB/cm. Electro-optic modulation has been demonstrated with Vπ = 6.3 V at a wavelength of 633 nm and Vπ = 9.5 V at a wavelength of 1550 nm for the aaxis samples and with Vπ = 8 V at 633 nm wavelength and Vπ = 15 V at 1550 nm for the c-axis samples. Modelling of the modulators gave the Pockels coefficient r51 = 80 pm/V for the c-axis film and an effective Pockels coefficient reff =734pm/V for the a-axis films at 633nm wavelength.