AbstractDeveloping intelligent electromagnetic wave (EMW) absorption materials with real‐time response‐ability is of great significance in complex application environments. Herein, highly compressible Fe@CNFs@Co/C elastic aerogels were assembled through the electrospinning method, achieving EMW absorption through pressure changes. By varying the pressure, the effective absorption bandwidth (EAB) of Fe@CNFs@Co/C elastic aerogels shows continuous changes from low frequency to high frequency. The EAB of Fe@CNFs@Co/C elastic aerogels is 14.4 GHz (3.36–17.76 GHz), which covers 90% of the range of S/C/X/Ku bands. The theoretical simulation indicates that the external pressure prompts a reduction in the spacing between the fiber layers in the aerogels and facilitates the formation of a 3D conductive network with enhanced attenuation ability of EMW. The uniform distribution of metal particles and appropriate layer spacing can effectively optimize the impedance matching to achieve the best EMW absorption performance. This work state clearly that the hierarchically assembled elastic aerogels composed of metal–organic frameworks (MOFs) derivatives and carbon fibers are ideal dynamic EMW absorption materials for intelligent EMW response.image