As a self-powered device, triboelectric fiber-generators (TEFGs) have garnered considerable attention over the past decade, overcoming the limitations of conventional power sources. Significantly, while both structures function, the aligned nanofiber film demonstrably outperforms the random nanofiber film in triboelectric output performance. Hence, a triboelectric all-nanofiber generator with an aligned structure is investigated, consisting of the co-electrospun polyacrylonitrile (PAN)/thermoplastic polyurethane (TPU) nanofiber positive triboelectric layer and polyvinylidene fluoride (PVDF)/polydimethylsiloxane (PDMS) nanofiber negative triboelectric layer. After the optimization of structure, triboelectric fiber-generators with aligned (A-TEFG) exhibited peak-to-peak voltage, current output, and transient power density values of 55 V, 0.8 μA, and 33.6 mW/m 2, respectively, which could efficiently harvest mechanical energy to power light-emitting diodes (LEDs). Furthermore, A-TEFG was used as self-powered sensors for human movement monitoring and transmitting encrypted information followed Morse code principles. Based on the simple and scalable fabrication methods, A-TEFG makes a promising candidate to developing practical, flexible, and self-powered wearable electronic devices.