Polylactide (PLA) is a biodegradable thermoplastic widely used in different fields, but it should be adequately modified considering high-performance applications. However, the current processes for developing PLA materials achieve high strength at the expense of toughness or ductility of the materials. Therefore, there is need to develop new strategies for generation of PLA materials with high strength, great toughness, good ductility, and high heat resistance. The present study reported a facile and cost-effective structural manipulation strategy for fabricating high-performance PLA composites that involved addition of 0.5 wt% self-assembled nucleation agent (TMC-306). During the structural manipulation process, the nucleation agent (TMC-306 shish) initially induced the PLA materials to develop a random shish-kebab crystal structure. A chain-like interlocking shish-kebab crystal structure with gradients in both length and thickness was then achieved through semi-solid high-pressure molding. The resulting super-PLA product showed excellent tensile strength (98.7 MPa), superb toughness (82.7 kJ/m²), and high elongation at break (117.5%). The reported qualities of the super-PLA materials were superior to that of most commercially available commodity polymers and were comparable to engineering plastics. In addition, PLA composites exhibited a lower thermal deformation variable and a higher Vicat softening temperature (112.4 °C) than neat PLA (62.1 °C). The facile strategy reported in the present study allows development of strong, tough, ductile, and thermally stable PLA, making it a potential alternative plastic material to commodity and engineering plastics used in many technical fields.

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