Recent advancements in printing technologies allow for fabricating various wearable sensors, circuits, and integrated electronics. However, most printing tools have limited ranges of handling ink viscosity, a short working distance, and a limited feature size for developing sophisticated electronics. Here, this paper introduces an all-in-one integrated wearable electronic system via multilayer, multinanomaterial printing. Versatile, highresolution aerosol-jet printing could successfully print Cu nanoparticles, Ag nanoparticles, PEDOT:PSS, and polyimide (PI) to manufacture nanomembrane composite structures, including skincontact electrodes and wireless circuits. The printed polymer, PEDOT:PSS deposited on the Cu, ensures biocompatibility when making direct skin contact while enhancing electrical conductivity for electrodes. A self-assembled monolayer facilitates better adhesion of Cu nanoparticles on the PI. Also, using intensive pulsed light, a photonic sintering method minimizes Cu-oxidation while avoiding thermal damage. The combined experimental and computational study shows the mechanical flexibility and reliability of the printed integrated device. With human subjects, the flexible wireless bioelectronic system demonstrates superior performance in detecting high-fidelity physiological signals on the skin, including electromyograms, electrooculograms, electrocardiograms, and motions, proving its potential applications in portable human healthcare and persistent human−machine interfaces.