Multiferroic 0.6BaTiO3-0.4NiFe2O4dense nanoceramic composites were synthesized via a powder-in-sol precursor hybrid chemical synthesis route and a ceramic sintering process. At the measured frequency range (1 kHz~1 MHz), the relative dielectric constant is 150~1670 and the dielectric loss is 0.05~0.70. The composite ceramic showed obvious coexistence of ferroelectric and ferromagnetic phases. With the increase of temperature, the saturation ferromagnetic magnetization decreases, while the ferroelectric polarization increases.