Dynamic nuclear polarization (DNP) is used in nuclear magnetic resonance to transfer polarization from electron spins to nuclear spins. The resulting nuclear polarization enhancement can, in theory, be two or three orders of magnitude depending on the sample. In solid-state systems, however, there are competing mechanisms of DNP, which, when occurring simultaneously, reduce the net polarization enhancement of the nuclear spin. We present a simple quantum description of DNP and apply optimal control theory (OCT) with an open-quantum-system framework to design pulses that select one DNP process and suppress the others. We demonstrate experimentally an order of magnitude improvement in the DNP enhancement using OCT pulses.