Multiferroics with strong magnetoelectric coupling can be created by improving the magnetostriction of the ferrite phase and combining it with the best-known piezoelectric. Herein, the ferromagnetic CoFe2O4 was modified with Al incorporation further improve the resistivity, magnetic, and magnetostrictive properties and then combined with (0.5)Ba(Zr0.2Ti0.8)O3−(0.5)(Ba0.7Ca0.3)TiO3 (BCZT) with different weight percentages. XRD results revealed the presence of a mixed spinel cubic phase for CAF (Fd-3m), whereas BCZT crystallized in a tetragonal structure (Amm2) in composite systems. The dielectric response of the materials was studied using impedance spectroscopy and it displayed a typical Maxwell–Wagner polarization of two-phase composites. The magnetic response of the CAF sample improved significantly which is attributed to the preference of Al3+ ions on tetrahedral sites. The magnetization of composites increased as the nonmagnetic BCZT component increased and the (0.75)CAF-(0.25)BCZT system had the highest saturation magnetization. We anticipate that these systems will have significantly improved magnetoelectric characteristics than unmodified CFO-BCZT systems.