We investigate the growth phase diagram of pseudobrookite Fe2TiO5 epitaxial thin films on LaAlO3 (001) substrates using pulsed laser deposition. Control of the oxygen partial pressure and temperature during deposition enabled selective stabilization of (100)- and (230)-oriented films. In this regime, we find an optical gap of 2.1 eV and room temperature resistivity in the range of 20–80 Ω cm, which are significantly lower than α-Fe2O3, making Fe2TiO5 potentially an ideal inexpensive visible-light harvesting semiconductor. These results provide a basis to incorporate Fe2TiO5 in oxide heterostructures for photocatalytic and photoelectrochemical applications.