Anchoring Nanofillers at Immiscible Polymer Interfaces Enables Strong, Tough, High-Output Triboelectrics

Triboelectric nanogenerators (TENGs) are promising for self-powered wearable electronics, but simultaneously achieving high mechanical performance and triboelectric efficiency in biobased polymers remains challenging. Poly(lactic acid) (PLA) and poly(butylene succinate) (PBS) offer complementary mechanical characteristics yet suffer from poor miscibility, limiting their effectiveness in TENGs. Here, we present a scalable interfacial-anchoring strategy that uses Pickering-emulsion-assisted melt blending to localize carbon-based nanofillers─carbon black (CB), carbon nanotubes (CNTs), and graphene nanoplatelets (GNPs)─at the PLA/PBS interface. With only 1 wt % loading, this approach enhances strength, toughness, and triboelectric output. CNT localization enables efficient stress transfer, yielding a 12.0% increase in tensile strength, a 7.1-fold increase in elongation at break, and a peak power density of 996.4 mW·m–2. Mechanistic analysis attributes these improvements to interfacial polarization, with the apparent dielectric constant increasing by up to 205-fold. The composite films operate stably and are suitable for wearable power generation and sensing.