Electromagnetic (EM) absorbers play an increasingly essential role in the electronic information age, even toward the coming “intelligent era”. The remarkable merits of heterointerface engineering and its peculiar EM characteristics inject a fresh and infinite vitality for designing high‐efficiency and stimuli‐responsive EM absorbers. However, there still exist huge challenges in understanding and reinforcing these interface effects from the micro and macro perspectives. Herein, EM response mechanisms of interfacial effects are dissected in depth, and with a focus on advanced characterization as well as theoretical techniques. Then, the representative optimization strategies are systematically discussed with emphasis on component selection and structural design. More importantly, the most cutting‐edge smart EM functional devices based on heterointerface engineering are reported. Finally, current challenges and concrete suggestions are proposed, and future perspectives on this promising field are also predicted.

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The exploration of ultra-wideband electromagnetic shielding materials is still a huge challenge to eliminate electromagnetic interference from various frequencies electronic devices in military and civil fields. Herein, a free-standing graphene...