Poly(Lactic Acid)/ TMC ‐306 Composite Films With Tailored Structure by Biaxial Stretching

Incorporating nucleating agents represents the most straightforward approach to enhancing the crystallization of polylactic acid (PLA), effectively improving crystallization kinetics and morphological control. However, achieving significant crystallization within the short time frames typical of industrial processing remains a challenge. In this work, we demonstrate a synergistic strategy combining the nucleating agent tetramethylene‐dicarboxylic dibenzoyl‐hydrazide (TMC‐306) as a crystallization template with biaxial stretching to facilitate the crystallization of PLA. By optimizing extrusion casting parameters and applying biaxial stretching, the PLA/TMC‐306 composite films achieved a crystallinity of 39.29%, a tensile strength of 101.92 MPa, an elongation at break of 83.00%, and a toughness of 72.23 MJ/m 3 . These values represent increases by approximately 9.61, 1.75, 13.13, and 31.54 times, respectively, compared to those of pure PLA films. More importantly, TMC‐306 templates serve as nucleation sites, reorganizing into dendritic superstructures and promoting the formation of a distinctive shish‐kebab‐like structure within the PLA matrix during biaxial stretching, which contributes to the superior performance of the composites. This work offers a viable and industrially scalable strategy for producing high‐performance sustainable plastic film.