We investigated the microstructure, crystal structure, dielectric, and elecromechanical strain properties of lead-free BaTiO3 (BT)-modified (Bi1/2Na1/2)TiO3-SrTiO3 (BNT-ST) piezoelectric ceramics. Samples were prepared by a conventional ceramic processing route. Temperature dependent dielectric properties confirmed that a phase transition from a nonergodic relaxor to an ergodic relaxor was induced when the BT concentration reached 1.5 mol%, interestingly, where the average grain size reached a maximum value of 4.5 μm. At the same time, enhanced electromechanical strain (Smax/Emax = 600 pm/V) was obtained. It is suggested that the induced ferroelectric-relaxor phase transition by the BT modification is responsible for the enhancement of electromechanical strain in 1.5 mol% BT-modified BNT-ST ceramics.