4D printing is a newly emerging technique that shows the capability of additively manufacturing structures whose shape, property, or functionality can controllably vary with time under external stimuli. However, most of the existing 4D printed products only focus on the variation of physical geometries, regardless of controllable changes of their properties, as well as practical functionality. Here, a material combination concept is proposed to construct 4D printed devices whose property and functionality can controllably vary. The 4D printed devices consist of conductive and magnetic parts, enabling the integrated devices to show a piezoelectric property even neither part is piezoelectric individually. Consequently, the functionality of the devices is endowed to transfer mechanical to electrical energy based on the electromagnetic introduction principle. The working mechanism of 4D printed devices is explained by a numerical simulation method using Comsol software, facilitating further optimization of their properties by regulating diverse parameters. Due to the self‐powered, quick‐responding, and sensitive properties, the 4D printed magnetoelectric device could work as pressure sensors to warn illegal invasion. This work opens a new manufacturing method of flexible magnetoelectric devices and provides a new material combination concept for the property‐changed and functionality‐changed 4D printing.