Dense 0.6(Bi0.9La0.1)(Ga0.05Fe0.95)O-3-0.4(Pb1-xBax)TiO3(BLGF-PBT,x = 0, 0.1, 0.2, 0.3, and 0.4) ceramics with different Ba contents were prepared by the solid-state reaction method, and effects of Ba contents on the structure and multiferroic properties were investigated. X-ray diffraction results indicate that the Ba-modified BLGF-PBT ceramics exhibit single perovskite structure without detectable secondary phases, and a transition from tetragonal phase to rhombohedral one takes place with the increase of Ba content. The piezoelectric constantd(33), remanent polarizationP(r), and remanent magnetizationM(r)are improved by the Ba substitution simultaneously. Values ofP(r),M-r, andd(33)of BLGF-PBT ceramics for the composition ofx = 0.3 with the coexistence of tetragonal and rhombohedral phases are 20 mu C/cm(2), 0.05 emu/g, and 256 pC/N, respectively, much higher than those without Ba modification. The significantly improvedd(33)andM(r)indicate that BLGF-PBT ceramics with Ba modification provide alternative materials for multifunctional devices.