Multiferroic composites with the composition (1-x) BaTi0.8Sn0.2O3-(x) La0.5Ca0.5MnO3 (x =0, 0.3, 0.5, 0.7, 0.9 and 1) were prepared by sol-gel techniques. Rietveld refinements of the composites with 0-3 and 3-0 type connectivities exhibit the formation of pure phases and confirm the fraction of the composite samples. It was found that the composites grain size decreases slightly with increasing the La0.5Ca0.5MnO3 content. Magnetic measurements of the composite ceramics exhibit a gradual increase in saturation and remanent magnetization with increasing La0.5Ca0.5MnO3 content. Dielectric data demonstrate that the composite materials show high values of the dielectric constant in comparison with the parent compound BaTi0.8Sn0.2O3 (BTSO). In addition, an attempt is made to measure the magnetoelectric coupling coefficient and to explain the negative permittivity and losses occurring in these materials at a certain frequency and temperature conditions.