Single phase Cr1.3Fe0.7O3 has been successfully prepared by wet chemical method, accompanied by the surface morphology with pure diamond shaped structure of corundum and uniform grain growth. The splitting of magnetization curves at ∼220 K during varying temperature measurement indicates the magnetocrystalline anisotropy with the coexistence of antiferromagnetic and ferromagnetic phases. The obvious dielectric relaxation behavior has been determined above ∼125 K with the activation energy of 0.0318 eV, which is attributed to the dipolar relaxation caused by short-range polaron range hopping in the magnetic grains. The arresting magnetoelectric coupling effect near room temperature is certified in Cr1.3Fe0.7O3 from ∼125 K, with the maximum coupling coefficient of 5 % at ∼212 K. These characteristics mean that the sample has potential application value in fields such as spintronics devices and magnetoelectric memories.