While wearable self-powered electronic devices have shown promising improvements, substantial challenges persist in enhancing their electrical output and structural performance. In this work, a working mechanism involving simultaneous piezoelectric and triboelectric conversion within a monolayer-structured membrane is proposed. Single-layer binary fiber nanocomposite membranes (SBFNMs) (PVDF/CNT_X@PAN/CNT_X, DPCPC_X) with two distinct interpenetrating nanocomposite fibers were created through co-electrospinning, incorporating multiwalled carbon nanotubes (CNTs) into polyvinylidene fluoride (PVDF) and polyacrylonitrile (PAN), respectively. The resulting membrane demonstrated an exceptional synergistic effect of piezoelectricity and triboelectricity along with a high machine-to-electric conversion capability. The addition of CNTs increased the PVDF β-phase and the PAN planar zigzag conformation. As a result, the DPCPC_0.5-SBFNMs-based piezoelectric nanogenerator exhibited excellent electrical output (187 V, 8.0 μA, and 1.52 W m^-2), maintaining an exceptionally high level of output voltage compared with other piezoelectric nanogenerators. It successfully illuminated 50 commercial light-emitting diodes simultaneously. The output voltage of DPCPC_0.5-SBFNMs was 5.1 and 4.6 times higher than that of PAN or PVDF single-fiber membranes, respectively. Furthermore, the peak voltage of DPCPC_0.5-SBFNMs exceeded that of co-electrospinning PVDF/CNT_1.0@PAN (DPCP_1.0) and PVDF@PAN/CNT_1.0 (DPPC_1.0) by 20 and 10 V, respectively. The piezoelectric sensor made of DPCPC_0.5-SBFNMs accurately sensed human movement, ranging from tiny to large, and demonstrated utility as an alarm in medical treatment, fire fighting, and monitoring. Endogenous triboelectricity is proposed in SBFNM piezoelectric materials, enhancing electromechanical conversion and electrical output capacity, thereby promising a wide application potential in self-powered wearable electronic devices.

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