DNA and proteins fold in three dimensions (3D) to enable functions that sustain life. Emulation of such reversible folding schemes for functional materials can create promising opportunities for advancing a wide range of technologies. In particular, morphing 3D mesostructures via multiple dimensions for high-performance materials including monocrystalline silicon can enable unconventional designs in sensory robotics, biomedical devices, microelectronics, and microelectromechanical systems. Existing approaches to morphing functional materials mostly rely on planar processes, which often complicates needed mechanisms for structural reconfiguration and limits the choice of materials composition and dimension. This presentation will introduce a bioinspired microfolding strategy to realize 3D reconfigurable microelectronic systems in freestanding forms with various advanced materials and complex architectures. The microfolding mechanism allows access to any transitional states of the folded 3D structures in a reversible fashion, to modulate functionalities on demand. Demonstrations on microantennas for telecommunication, wearable accelerometers for tremor monitoring, and epicardial bioelectronic probes for cardiac mapping, all of which are achieved via the microfolding strategy, further highlight the high potential for a broad range of applications in healthcare and communications industry.