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A single device with a variety of capabilities is highly attractive for the increasing demands of complex and multifunctional optoelectronics. A hybrid heterojunction formed between CsPbBr3 halide perovskite and chalcogenide quantum dots is demonstrated. The heterojunction served as an asymmetric active layer allows not only charge separation/exciton dissociation in a benign process, but also carrier injection/recombination with the suppression of bulk and interfacial nonradiative recombination. An individual device incorporating such a heterojunction is therefore implemented with an integration of proof‐of‐concept functions, including a voltage controllable multicolor light‐emitting diode, an exceptionally high photovoltage energy‐harvesting device, and an ultrafast photosensitive detector. The figures of merit of the light‐emitting diode remarkably surpass those of the corresponding single‐active‐layer device, particularly in terms of its bright electroluminescence and superior long‐term stability. The asymmetric active layer concept provides a feasible route to design efficient multifunctional and monofunctional devices in the future. [ABSTRACT FROM AUTHOR]