Multifunctional flexible emergent triboelectric nanogenerators (TENGs) have garnered significant attention as efficient mechanical energy harvesters for wearable clothing applications. However, challenges persist in seamless integration intelligent clothing platforms while simultaneously achieving high-output signals, electromagnetic shielding, temperature regulation. In this study, the multifunctional wearable smart leather collagen fiber (S-LCF) based on natural leather collagen fibers (LCF) is cross-linked with Polyionic liquids, MOF-LDH composite materials (PILs/MOF-LDH-Zr) and is nanoengineered through PPy conducting network. As a positive triboelectric layer of multifunctional smart collagen fiber based triboelectric nanogenerators (SL-TENGs), S-LCF possesses a natural synaptic structure and achieves a power density of 795 mW m −2 and a sensitivity of 0.25 V·kPa −1. Additionally, S-LCF also exhibites exceptional electromagnetic shielding properties (SE T = 58 dB), photothermal performance (Standard solar density, 600 s, temperature rise to 81 °C), and antibacterial efficacy (over 99 % inhibition rate). As wearable smartclothes, S-LCF also demonstrates outstanding resistance to humid-thermal conditions, high mechanical strength, and excellent water vapor permeability. With its versatile capabilities, S-LCF holds immense potential for human-machine interfaces, and artificial intelligence applications, offering a multifunctional platform for the development of high-performance, on-demand wearable flexible electronic devices.