Lead-free multiferroic particulate composites of Ni0.83Co0.15Cu0.02Fe1.9O4-δ–Na0.5Bi0.5TiO3 (NCCF–NBT) ceramics are synthesized by spark plasma sintering in conjunction with high-energy ball milling. The exhibition of ferromagnetic and ferroelectric characteristics demonstrates that these materials are multiferroic in nature. Magnetic measurements indicate that the composites exhibit an excellent combination of saturation magnetization and coercivity at room temperature. In addition, they have a large magnetoelectric voltage sensitivity, which is up to 663mVcm−1Oe−1 under a magnetic field of 5kOe for the 0.5NCCF–0.5NBT composite.