Triboelectric tactile sensing technique is increasingly coming into people’s lives to bring convenience, so that there is an urgent necessity for this technique to be applied to smart mobility to increase safety and enhance the mobility experience. Herein, a single-electrode mode multilayer triboelectric sensor (MTS) motivated by artificial intelligence (AI) is proposed, which consists of styrene-butadiene-styrene (SBS)/ poly (vinylida-ene fluoride-trifluoroethylene) (PVDF-TrFE) nanofibers (NFs) film as the friction layer and substrate, laser-induced graphene (LIG)/molybdenum disulfide (MoS2) as the charge trapping layer, and Ag as the electrode. The MTS exhibits remarkable sensing performance, such as a wide response range of 5–100 N, 0.4–2 Hz multi-frequency response capability, and non-contact sensing, as well as distinguished self-powered performance. To demonstrate the practical significance of the proposed MTS, two applications are explored specifically after equipping with AI, including: (i) a smart in-vehicle system is constructed, which consists of unlocking section and multifunctional control with early warning section. (ii) a smart car control system is implemented, which can carry out special tasks instead of humans. These applications provide reliable ways to promote the development of human-machine interaction and smart mobility, as well as help to make lifestyles and mobility smarter, safer and more convenient.