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Most electronic skins (e-skins) show unique performance or possess sensory functions. The raw materials used for their preparation are potentially toxic or harmful, and there may be problems such as poor compatibility between the conductive fillers and polymers. In this paper, a silver-loaded nanocomposite film (PVA/CMS/vanillin/nanoAg) was prepared by the in situ reduction method in a greener route. The mechanical properties of this nanocomposite film had improved with a tensile strength of 30.95 MPa, an elongation at break of 101.9%, and a Young’s modulus of 10.62 MPa. In the composite matrix, a cross-linked network was constructed based on the coordination and hydrogen bonds, which was conducive to the stability of the reduced AgNPs and AgNWs. When applied as an e-skin in humidity/sweat sensors and wearable electronics, the nanocomposite film responds to humidity within 60 s and records the electric signals of human joint movements and skin sweating with a response range of 0–140% to strain at 93% RH. This kind of e-skin has excellent antibacterial and antioxidant activities and shows an outstanding ultraviolet-proof performance, which provides a greener promising reference route for the design of wearable e-skins to monitor the health and movements of humans.