Soft actuators with controllable responsiveness have wide application prospects in human-machine interfaces and intelligent robotics. However, the increasing integration and multi-functionality inevitably accumulate heat and radiate electromagnetic waves in electron components, detrimental to device service life and human health. Herein, cellulose nanofibers (CNFs)-based composites with excellent thermal conductivity (TC) and superior electromagnetic interference shielding efficiency (EMI SE) are prepared by layered dispersion of polyamide epichlorohydrin modified graphene nanosheets (pGNPs) within silver nanoparticles deposited CNFs through electrostatic self-assembly via vacuum filtration. The subsequent hot-pressing forms densely interconnected pGNPs within the CNFs-based composites with “mimosa”-like ordered layered architectures, showing a TC of 150.6 W/(m K) and an EMI SE of 75 dB. By integrating the CNFs-based composites with outstanding Joule heating performance into liquid crystal elastomers, smart curtains and intelligent grabbers are yield with a bending angle of 82° under a voltage of 3 V. Furthermore, the CNFs-based composite with an excellent conductivity (9.8 × 103 S m−1) is used as an electrode to construct triboelectric nanogenerators for transmitting information through Morse code. Overall, the as-prepared CNFs-based composites can be used to prolong the life of actuators and sensors, paving the way for multi-functional wearable terminals and biomimetic actuators.