Multiferroic materials that display a coexistence of ferroelectric and ferromagnetic responses attract interest because of their potential for several novel device applications. In multiferroic composite, electromagnetic coupling is facilitated by elastic interaction between ferroelectric and ferromagnetic components via piezoeffect and magnetostriction. The goal of our research is to prepare magnetoelectric composite using sol-gel technology. This method consisted of two steps, preparing a mixture of the synthesized ferromagnetic and ferroelectric nanoparticles at certain ratio and sintering. The nanoparticles were characterized by Differential Thermal Analysis and Thermogravimetric Analysis. The crystal structure and microstructure were studied by X-ray Diffraction and Scanning Electron Microscopy, respectively. Dielectric Analysis, Superconducting Quantum Interference Device and Vibrating Sample Magnetometer were used to examine the electric and magnetic properties. BTO-CFO multiferroics whose electric permittivity increased by magnetization were successfully synthesized by this method.