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Abstract 2D black phosphorene (BP) carries a stellar set of physical properties such as conveniently tunable bandgap and extremely high ambipolar carrier mobility for optoelectronic devices. Herein, the judicious design and positioning of BP with tailored thickness as dual‐functional nanomaterials to concurrently enhance carrier extraction at both electron transport layer/perovskite and perovskite/hole transport layer interfaces for high‐efficiency and stable perovskite solar cells is reported. The synergy of favorable band energy alignment and concerted cascade interfacial carrier extraction, rendered by concurrent positioning of BP, delivered a progressively enhanced power conversion efficiency of 19.83% from 16.95% (BP‐free). Investigation into interfacial engineering further reveals enhanced light absorption and reduced trap density for improved photovoltaic performance with BP incorporation. This work demonstrates the appealing characteristic of rational implementation of BP as dual‐functional transport material for a diversity of optoelectronic devices, including photodetectors, sensors, light‐emitting diodes, etc.more » « less
