Smart electromagnetic functional devices prepared based on electromagnetic wave responsive materials will provide more convenience for human life in the future. Here, we prepare oriented magnetic liquid metal droplet-filled polydimethylsiloxane films with micropillar array patterned surfaces, and further assemble them into bilayer films with interlocked structures. Once compressed, the increase in conductivity of the film due to the tunneling effect between microarrays and the elongation of liquid metal droplets leads to a rapid increase in electromagnetic interference shielding performance. Accordingly, a tunable electromagnetic interference shielding material with high sensitivity and wide control range is obtained, which has potential applications in electromagnetic wave control systems and intelligent electromagnetic protection systems. Meanwhile, we assemble a strain sensor and a magnetic sensor, which can precisely sense pressure and magnetic field according to changes in electromagnetic signal and electrical signal, respectively.