Ferroelectric solid solutions with composition near the morphotropic phase boundary (MPB) have gained extensive attention recently due to their excellent ferroelectric and piezoelectric properties. Here, we have demonstrated a strategy to realize the controllable preparation of BiFeO3-BaTiO3 (BF-BT) epitaxial films near the MPB. A series of high-quality BF-BT films were fabricated by pulsed laser deposition via adjusting oxygen partial pressure (PO2) using a BF-BT ceramic target. A continuous transition from rhombohedral to tetragonal phase was observed upon increasing PO2. Particularly, the film with a pure tetragonal phase exhibited a large remnant polarization of ∼90.6 μC/cm2, while excellent piezoelectric performance with an ultrahigh strain (∼0.48%) was obtained in the film with coexisting rhombohedral and tetragonal phases. The excellent ferroelectric and piezoelectric properties endow the BF-BT system near the MPB with great application prospects in lead-free electronic devices.