Using the free (pressureless) sintering method, multiferroic ceramic composites based on two ferroelectric materials, i.e., BaTiO3 (B) and Pb0.94Sr0.06 (Zr0.46Ti0.54)0.99Cr0.01O3 (P), and magnetic material, i.e., zinc–nickel ferrite (F) were obtained. Three composite compositions (BP-F) were obtained with a constant 90/10 content (ferroelectric/magnetic) and a variable content of the ferroelectric component (B/P), i.e., 70/30, 50/50, and 30/70. Crystalline structure, microstructural, DC electrical conductivity, dielectric, and ferroelectric properties of multiferroic composites were investigated. The concept of a composite consisting of two ferroelectric components ensures the preservation of sufficiently high ferroelectric properties of multiferroic composites sintered by the free sintering method. Research has shown that the percentage of individual ferroelectric components in the composite significantly affects the functional properties and the entire set of physical parameters of the multiferroic BP-F composite. In the case of the dielectric parameters, the best results were obtained for the composition with a more significant amount of BaTiO3; i.e., permittivity is 1265, spontaneous polarization is 7.90 µC/cm2, and remnant polarization is 5.40 µC/cm2. However, the most advantageous set of performance parameters shows the composite composition of 50BP-F.