Magnetoelectric (ME) materials that exhibit simultaneous coupling between electric polarization and magnetization have attracted significant attention due to their potential technological applications in the emerging generation of multifunctional devices. In this research, Ba_0.85Ca_0.15Ti_0.92Zr_0.08O₃-CoFe₂O₄:x (x = 0.1, 0.2, 0.3% mol) composites were synthesized using solid-state and sol–gel combustion chemical methods to elucidate their ME coupling at ultra-low concentrations of the magnetic phase. Rietveld refinement and Raman spectroscopy results confirm a shift in the morphotropic phase boundary (MPB), evidenced by an increase in the tetragonal phase relative to the orthorhombic structure. High stability of the P4mm and Amm2 symmetries is reached at 1300 °C without diffusion of Fe and Co into the octahedral site. At this temperature, the CoFe₂O₄ spinel structure remains stable without secondary phases. The orthorhombic phase fraction decreases from 55% to 37% as the magnetic phase fraction increases, driven by stress and constraint rather than ionic interactions alone. The Curie temperature decreases from 99 to 90 °C, attributed to the grain-size reduction effect rather than structural disorder. The dielectric permittivity (ε_r) reaches an absolute value of 5070 and progressively decreases with increasing magnetic saturation. An increase in compressive residual stress is observed, which ensures the mechanical stability of the electroceramics. Magnetoelectric (ME) coupling, evaluated through measurements of electric polarization as a function of the magnetic field, shows an increase from 3.8 to 4.9 μC/cm² under a magnetic field of 50 Oe. The composites with x = 0.2 and 0.3 mol% exhibit potential for applications in fast-switching magnetoelectric devices and magnetic field sensors.