The 0.96Na_(0.5)Bi_(0.5)TiO_(3)-0.04K_(0.5)Bi_(0.5)TiO_(3)(NKBT96/4)lead-free single crystal was successfullygrown by top-seeded solution growth method.The effective segregation coefficient for K was calculated to be 0.20.X-ray powder difraction measurement showed that the as-grown crystalpossesses rhombohedral perovskite structure at room temperature.X-ray rock curve measureindicated that the as-grown single crystal owned relatively higher quality.The NKBT96/4 singlecrystal exhibits apparent diffused dielectric behavior,where the diffusiveness index aαis 1.79 forthe[001]-oriented crystal planes.A notable thermal hysteresis,△T_(h),of 25℃was disclosed for thetetragonal antiferroelectric-tetragonal paraelectric phase transition in the dielectric propertystudies between heating and cooling.The highest remnant polarization,P_(r),16.8μC/cm^(2),wasobtained at 100℃.The electromechanical coupling coefficient k_(t)of the[001]-oriented crystalplanes at room temperat ure was determined to be 38%using resonance-antiresonance technique.The room temperature piezoelectric constant d_(33)reaches 120 pC/N.