Magnetoelectric (ME) ceramic composites of CoFe2O4 (CFO) and BaTiO3 (BTO) were prepared by spark plasma sintering. The CFO/BTO ceramic composites with fine microstructures exhibited a significant improvement in the ME voltage coefficient reaching up to 0.18 V/cm Oe. A perfect ME anisotropy was also observed in the CFO/BTO ceramic composites which consisted well with the fitted curve. The enhanced ME voltage coefficient alone with the perfect ME anisotropy in these ceramic composites provides a possibility of developing a magnetic field sensor capable of probing the strength as well as the direction of an unknown magnetic vector.