The doublet-spin nature of radical emitters is advantageous for applications in organic light-emitting diodes (OLEDs), as it avoids the formation of triplet excitons that limit the electroluminescence efficiency of non-radical emitters. However, radicals generally show low optical absorption and photoluminescence yields. Here we explain the poor optical properties of radicals based on alternant hydrocarbons, and establish design rules to increase absorption and luminescence yields for donor-acceptor-type radicals. We show that non-alternant systems are necessary to lift the degeneracy of the lowest energy orbital excitations; moreover, intensity borrowing from an intense high-lying transition by the low energy charge-transfer excitation enhances the oscillator strength of the emitter. We apply these rules to design tris[2,4,6-trichlorophenyl] methyl (TTM)-pyridoindolyl derivatives with high photoluminescence quantum yield (>90%). OLEDs based on these molecules showed pure-red emission with over 12% external quantum efficiency. These insights may be beneficial for the rational design and discovery of highly luminescent doublet emitters.