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High-performance lead-free multiferroic composites are desired to replace the lead-based ceramics in multifunctional device applications. Laminated compounds were prepared from ferroelectric and ferromagnetic materials. In this work, we present the laminated ceramics compound by considering the ferromagnetic La 0.5 Ca 0.5 MnO 3 (LCMO) and the ferroelectric BaTi 0.8 Sn 0.2 O 3 (BTSO) in two different proportions. Compounds ( 1-x ) LCMO-( x ) BTSO with x = 1 and 0 (pure materials) were synthesized by the sol-gel method, and x = 0.7 and 0.5 (laminated) compounds were elaborated by welding appropriate mass ratios of each pure material by using the silver paste technique. Structural, dielectric, ferroelectric, microstructure, and magnetic characterizations were conducted on these samples. X-ray scattering results showed pure perovskite phases confirming the successful formation of both LCMO and BTSO. Scanning electron microscope (SEM) images evidenced the laminated structure and good quality of the interfaces. The laminated composite materials have demonstrated a multiferroic behavior characterized by the ferroelectric and the ferromagnetic hysteresis loops. Furthermore, the enhancement of the dielectric constant in the laminated composite samples is mainly attributed to the Maxwell-Wagner polarization.