Control of carrier transport in organic semiconductors by aluminum doping is realized in organic light-emitting devices (OLEDs) for which electroluminescence can sensitively reflect the status of carrier transport. It is found that an Al-doped layer with proper thickness (∼1–10nm) may block hole transport completely and enhance electron transport to some extent regardless of its location in the organic carrier transport layers. Improvement in the efficiency of OLEDs with an aluminum cathode is achieved upon the introduction of a very thin (∼3nm) Al-doped region near the light-emitting area. The current efficiency obtained with such Al-doped devices is about 30% higher than that with undoped devices.