With rapid advancements in the nuclear field, the development of an integrated protective-alarm platform for radioactive contamination is essential for safeguarding human health. Herein, NH2-UiO-66/chitosan crosslinked networks are incorporated into a graphene oxide/konjac glucomannan (GO/KGM) matrix to engineer aerogels (NCGK-X) featuring multifunctional binding sites and a hierarchically porous architecture for efficient iodine capture and sensing. The ternary synergistic aerogel enables rapid iodine diffusion while facilitating efficient capture at abundant adsorption sites throughout the matrix. Furthermore, by regulating the proportion of NH2-UiO-66@CS fillers, the interaction strength and kinetics of electron transfer between active sites and iodine molecules are optimized, and enhancing the polarization of iodine molecules. This electron transfer alters the surface electronic properties of the aerogel, thereby enabling NCGK-X's rapid triboelectric response to iodine. The optimized NCGK-7 achieves exceptional iodine capture (5.94 g/g vapor, 95.5% aqueous removal), while NCGK-4 enables rapid triboelectric sensing (3 s response). Leveraging dual functionalities, NCGK-7 serves in protective masks and NCGK-4 in threshold alarms, enabling real-time monitoring-protection synergy against iodine hazards. Overall, these multifunctional NCGK-X aerogels present promising prospects for nuclear safety management through synergistic contamination mitigation and environmental surveillance.