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Two-dimensional (2D) metal−organic frameworks (MOFs) play an essential role in response to external stimuli by changing their physical or chemical properties. This Review mainly aims at the recent progress of stimuliresponse in 2D MOFs. The various external stimuli, such as ions, solvents, gas, light, electron, temperature, and others, to 2D MOFs are systematically introduced and summarized. In addition, future perspectives relate to 2D MOFs for the stimuli-response are also discussed. We hope that this Review could provide a guideline to help researchers to design new stimuli-response 2D MOFs.

Two identical layered metal–organic frameworks (MOFs) (CoFRS and NiFRS) are constructed by using flexible 1,10‐bis(1,2,4‐triazol‐1‐yl)decane as pillars and 1,4‐benzenedicarboxylic acid as rigid linkers. The single‐crystal structure analysis indicates that the as‐synthesized MOFs possess fluctuant 2D networks with large interlayer lattices. Serving as active electrode elements in supercapacitors, both MOFs deliver excellent rate capabilities, high capacities, and longstanding endurances. Moreover, the new intermediates in two electrodes before and after long‐lifespan cycling are also examined, which cannot be identified as metal hydroxides in the peer reports. After assembled into battery‐supercapacitor (BatCap) hybrid devices, the NiFRS//activated carbon (AC) device displays better electrochemical results in terms of gravimetric capacitance and cycling performance than CoFRS//AC devices, and a higher energy‐density value of 28.7 Wh kg−1 compared to other peer references with MOFs‐based electrodes. Furthermore, the possible factors to support the distinct performances are discussed and analyzed.