Multifunctional electromagnetic wave (EMW) absorbing materials are attracting attention because of their potential applications in medical, livelihood, and military. In this study, a pomegranate‐like nanolayer featuring a core‐shell architecture (PNCS) is prepared using a confinement strategy. Introducing metal atoms into this unique pomegranate‐like design (M‐PNCS, M = Mn, Fe, Co, Ni, and Cu) effectively tuned the electromagnetic response and improved the electromagnetic functions. The Mn‐PNCS composite exhibited the highest electromagnetic absorption. Its reflection loss (RL) reached −62.39 dB with an effective absorption bandwidth (EAB) at 1.8 mm of 6.0 GHz. As the charge transport capacity of the Mn‐PNCS increases, its absorption can be transformed into shielding, with a green shielding index of up to 3.54. On this basis, Mn‐PNCS is used to fabricate a multifunctional film and a new design of strain sensor. This multifunctional film integrated electromagnetic absorption, thermal insulation, hydrophobicity, flexibility, and sensing, thus showing potential for use in wearable electromagnetic protective clothing. In addition, the sensors in the simulation design achieved strain sensing through the coupling effect between the Mn‐PNCS patterns. These findings demonstrate that Mn‐PNCS is an excellent multifunctional material with potential applications in the technical fields of EMW absorption, electromagnetic shielding, and wearable devices.