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The nanofiller zirconium phosphate (ZrP) was mixed into poly(lactic acid) (PLA) to ameliorate its thermal stability. The elastomer ethylene-methyl acrylate-glycidyl methacrylate copolymer (E-MA-GMA) was introduced into the PLA/ZrP nanocomposite through melt-mixing to improve its toughness and obtain a super-tough PLA/ZrP/E-MA-GMA nanocomposite. The impact strength of the PLA/ZrP/E-MA-GMA nanocomposite, with a composition ratio of 72/3/25, was improved to 71.5 kJ/m², about 25 times greater than the impact strength of pure PLA. The dynamic mechanical analysis (DMA) confirmed that E-MA-GMA has excellent compatibility with the matrix of PLA. A typical core–shell structure that can cause massive shear-yielding deformation was characterized by transmission electron microscopy (TEM), which gave the nanocomposite excellent toughness.