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Emerging organic light-emitting electronic devices such as organic light-emitting transistors and lasers need materials combining high luminescence and efficient charge transport. Doping of the materials by highly luminescent molecules is an efficient approach to control and enhance the material luminescence. Here, we introduce the concept of self-doping according to which a higher luminescent dopant emerges as a byproduct in the course of the host material synthesis, and demonstrate how the dopant controls the luminescent and charge transfer properties of organic semiconductor crystals.