Rapid development of modern wearable-implantable medical devices has led to research on mechanical energy harvesting technologies, especially triboelectric nanogenerator (TENG) for being sustainable/flexible power supply or self-powered sensor. The most challenge part is searching advanced materials and designing them with excellent electrical performance while being flexible, lightweight, and non-toxic. Layered double hydroxides (LDH) have sparked research interest owing to the facile tunability of composition, morphology, and physicochemical properties. In this work, magnesium aluminum layer double hydroxide (MgAl-LDH) nanosheets were employed as a dielectric filler dispersed onto bacterial cellulose (BC) matrix, prior to the application as a friction layer in TENG. Phase identification, functional groups, and morphology of the nitrate-intercalated MgAl-LDH layered crystals have been investigated, including the nanosheets (NS) colloid exfoliated therefrom in formamide. Mechanistic insight with a detailed discussion of experimental results linked to scientific theory is deeply explained. The optimized BC/MgAl-LDH NS (1.5%v/v) film, simply prepared by casting, delivers the open-circuit voltage (VOC), short-circuit current (ISC), and maximum output power (Pmax) of 88.5 V, 87.7 µA and 1250 µW (138 µW/cm2), respectively. The composite serves not only as a nanogenerator driving 200 LEDs but also as a self-powering sensor detecting finger movements that might be useful for developing trigger finger monitoring in future.