Magnetoelectric materials which simultaneously exhibit electric polarization and magnetism have attracted more and more attention due to their novel physical properties and promising applications for next-generation devices. Exploring new materials with outstanding magnetoelectric performance, especially the manipulation of magnetization by electric field, is of great importance. Here, we demonstrate the cross-coupling between magnetic and electric orders in polycrystalline Co4Nb2O9, in which not only magnetic-field-induced electric polarization but also electric field control of magnetism is observed. These results reveal rich physical phenomenon and potential applications in this compound.