© 2016 SPIE. We present a novel technique of efficient optical pumping of open, high-angular-momentum systems. The method combines two well-established approaches of population manipulation (conventional optical pumping and coherent population transfer), offering the ability to achieve higher population of a sublevel with the highest or lowest quantum number m (the "end state") than obtainable with either of the techniques. To accomplish this task, we propose to use coherent-population-transfer technique (e.g., adiabatic fast passage) to arrange the system in such a way that spontaneously emitted photon (conventional optical pumping) carries away more entropy than in conventional schemes. This enables reduction of a number of spontaneous decays Nsd required to pump the system with the total angular momentum J from Nsd = J decays in the conventional scheme to Nsd ≤ log2(2J) decays in the proposed scheme. Since each spontaneous-emission event is potentially burdened with a loss of population (population is transferred to a dark state), this enables increasing population accumulated in the "end state", which is important for many applications.