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Multiferroic materials have attracted significant research attention due to their technological potential for applications as multifunctional devices. The scarcity of single-phase multiferroics and their low inherent coupling between multiferroic order parameters above room temperature pose a challenge to their further applications. We propose a 3BiFeO3/7BaTiO3 perovskite–perovskite composite that combines ferroelectricity and ferromagnetism. We demonstrate that the sintering temperature can tailor the ferroelectricity and ferromagnetism of the composites. The multiferroicity can be achieved at a low sintering temperature in the composite-like structure ceramics, and its multiferroic properties, especially the ferromagnetism, are superior to those of solid solutions. We also investigate the dynamic evolution of multiferroicity with sintering temperature. We adopt a nano–micro strategy to construct a composite-like microstructure, which results in optimized ferroelectric (1.62 μC cm−2) and ferromagnetic (0.16 emu/g) characteristics at a sintering temperature of 750 °C. We also found experimental evidence of the competition between antiferromagnetic and ferromagnetic interactions in the transition metal cation sublattice. Multiferroic BiFeO3/BaTiO3 composites with combined ferroelectric and ferromagnetic properties have significant potential for various applications. [ABSTRACT FROM AUTHOR]