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Main characteristics of organic field effect transistors (OFETs) strongly depends on chemical structure and purity of organic semiconductors. Recently we introduced a novel concept of molecular self-doping, in which highly luminescent dopants emerges as minute-amount by-products during the host material synthesis. Molecular self-doping is advantageous for improved excitonic transport and host-dopant energy transfer in highly luminescent semiconducting organic single crystals for optoelectronics. Monolayer OFETs are promising due to their unique sensitivity to the environment, which allows creation of ultrasensitive gas sensors. Monolayer OFETs can be prepared either by physisorption or by self-assembly. The former are single-crystal monolayers of unprecedented structural order grown from solution by drop or spin casting with subsequent slow solvent evaporation, which demonstrated excellent performance in OFETs. The latter are highly stable organosilicon derivatives of organic semiconductors capable to self-assembly on the water-air interface, which allows to produce stable SAMFETs and ultrasensitive gas sensors based on them.