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We report the synthesis and study of the photoluminescence properties of colloidal lanthanide(III)-doped Ga2O3 nanocrystals. The Ga2O3 nanocrystal host lattice acts as a sensitizer of the Eu3+ dopant red emission arising from intra-4f orbital transitions, and concurrently exhibits a strong blue photoluminescence originating from defect-based donor–acceptor pair (DAP) recombination. The Eu3+ sensitization, enabled by the energy transfer from the nanocrystal host lattice to the dopant centers, allows for the generation of dual blue-red emission. Increasing doping concentration leads to a decrease in the donor activation energy allowing for simultaneous control of the optical and electrical properties of these multifunctional nanocrystals. Analyses of the steady-state and time-resolved photoluminescence spectra suggest that Eu3+ ions occupy at least two different sites, which were tentatively designated as the six …