The concurrent presence of large electric polarization and strong magnetoelectric coupling is quite desirable for protentional applications of multiferroics. In this paper, we report the growth of CdMn7O12 single crystals by flux method under a high pressure of 8 GPa for the first time. An antiferromagnetic (AFM) order with a polar magnetic point group is found to occur at the onset temperature of TN1 = 88 K (AFM1 phase). As a consequence, the pyroelectric current emerges at TN1 and gradually increases and reaches its maximum at Tset = 63 K, at which the AFM1 phase finally settles down. Below Tset, CdMn7O12 single crystal exhibits a large ferroelectric polarization up to 2640 µC/m2. Moreover, the spin-induced electric polarization can be readily tuned by applying magnetic fields, giving rise to considerable magnetoelectric coupling effects. Thus, the current CdMn7O12 single crystal acts as a rare multiferroic system where both large polarization and strong magnetoelectric coupling merge concurrently.