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A series of solid solution of (1− x)BiFeO- xBaTiO (abbreviated as BFO- xBT at 0.24 ≤ x ≤ 0.34) were prepared to reveal the relation between phase structure and multiferroic properties. A morphotropic phase boundary (MPB) separating R phase and T one was detected in BFO- xBT system at 0.26 ≤ x ≤ 0.34. Due to R and T two -phase coexistence, high piezoelectric properties of d = 191 pC/N and k = 34.68%, as well as excellent ferroelectric properties of 2 P = 56.13 μm/cm and 2 E = 75.35 kV/cm were achieved in the BFO- xBT ceramics at x = 0.30. Moreover, a low leakage current density ( J) of 1.01 × 10-3.18 × 10 A/cm at an applied electric field of 30 kV/cm and a weak ferromagnetism with remanent magnetization M of 0.014-0.054 emu/g and coercive fields H of 946-2340 Oe were detected in BFO- xBT ceramics at 0.24 ≤ x ≤ 0.34, suggesting that the BFO-BT ceramics have promising prospects in magnetoelectric functional components. [ABSTRACT FROM AUTHOR]