(1-x) BiFeO3–(x) CaTiO3 [(1-x) BFO – (x) CTO, (x = 0, 0.1, 0.2 and 0.3)] composites were synthesized using sol-gel chemical rout method. X-ray diffraction investigation shows the crystal structure changes from rhombohedral to monoclinic for 0 ≤ x ≤ 0.2, and it changes to orthorhombic at x ≤ 0.3. The Field Emission Scanning Electron Microscope (FESEM) investigation confirms the the microstructure consists of randomly oriented, homogenous, and non-uniform grains. The dielectric permittivity (ε) and tangent loss (tanδ) decreases with increasing frequency and show dielectric anomalies (as a hump) at different temperatures for different compositions. The incorporation of CTO, decreases three order of leakage current (up to x = 0.2) and significantly improve the magnetization and magneto-dielectric coupling. The frequency-dependent ac conductivity obeys Jonscher’s power law with large ac conductivity dispersion for higher frequencies with increasing CTO concentration. The variations of ac conductivity with the inverse of temperature obey the Arrhenius equation and show negative temperature coefficient of resistance (NTCR) behavior. The ferromagnetic (FM) properties in BFO-CTO increases significantly with an increase of the CTO concentration. The coercive field increases with increasing CTO concentration suggesting a competition between the antiferromagnetic and ferromagnetic ordering. At room temperature, all the samples show strong magneto-dielectric coupling.