Cellulosic triboelectric materials have gained widespread attention in triboelectric nanogenerators (TENGs) recently due to their fascinating merits of renewability, biodegradability, and low cost. However, cellulose-based TENGs still are challenged by the low surface charge density of triboelectric materials. Herein, the negative charged cellulosic triboelectric materials are functionalized as triboelectric layers for self-powered sensors via an electrostatic spinning method, where the electrospun polyvinylidene fluoride (PVDF) nanofibers fill with the porous air-laid paper (AP), boosting the formation of polar β-phase crystals and a negative shift of the surface potential. The TENG constructed with PVDF/12 wt%@AP affords charge output of 60.7 μC m