The exploitation of wearable electronic devices with diversified environmentally adaptivity, advanced additive manufacturing, efficient microwaves absorption, and self-powered sensing represents a pivotal strategic in promoting Artificial-Intelligence and personal electromagnetic safety. However, achieving robust multifunctional integration in a single flexible device is still an unprecedented challenge. Herein, the multidimensional and multiphase nanofiller with hierarchical structures and tailored defects, and comb/bottlebrush polysiloxane with multifluorination and multireversible bond, featuring dynamic interface interaction, are designeded. Subsequently, a dual-mode intelligent wearable sensor is assembled based on direct-ink-writing and electrostatic-spraying technology. The 3D-printed triboelectric nanogenerator (TENG) exhibited excellent triboelectric output (Voc = 185.4 V, Isc = 1576.2nA, power density = 729.8mW m−2) and durability in virtue of multi-scale roughness surface, interfacial polarization, efficient charge trapping, storage and transmission capacity. Accordingly, the fabric-based TENG is designed for demonstrating self-powered human activity monitoring and biomechanical energy harvesting. Benefiting from optimized impedance matching and multiple magnetic-dielectric coupling, the device exhibited exceptional personal electromagnetic protection behavior (RLmin = -64.81 dB, EAB = 5.1 GHz). Remarkably, the synergistic properties of superhydrophobic, oleophobic, and self-healing significantly improved reliability and life-span. This work presents as a proof-of-concept for an intelligent wearable device with extensive design-freedom, pioneering the integration of self-powered sensing, electromagnetic safety, and environmentally adaptivity, which will contribute to the development of high-quality human-machine interaction, wearable healthcare, and electronic skin.