Polylactic acid (PLA) is one of the most promising biodegradable materials, but poor toughness severely limits its application. Ionic liquids (ILs) have excellent plasticizing effects on PLA, but strength reduction and plasticizer precipitation remain worrisome. Herein, nanofibrillated cellulose (NFC), with excellent morphology, high modulus and strength, was prepared to reinforce PLA plasticization systems. Moreover, its numerous surface hydroxyl groups were tailored to bond with ILs, reducing plasticizer precipitation. The different sulfonation degrees of NFCs (low LSNFC, medium MSNFC, high HSNFC) and the influence of NFC amounts (0–7 wt%) on the mechanical, thermal and plasticizer precipitation properties of PLA composites were investigated. The results indicate that network-like C2/C3-sulfonated NFCs were successfully prepared through simple processing steps. Noteworthy, the tensile elongations of PLA composites increased with the addition of IL-XSNFC (all three degrees), with no significant reduction in tensile strength and modulus. The addition of 7 wt% IL-HSNFC resulted in an elongation of 25.01 % for PLA composites, which is 3.6 times that of pure PLA. Adding 3 wt% IL-MSNFC achieved ultra-high impact toughness of 3.19 kJ/m2, nearly double that of pure PLA. Interestingly, with increasing sulfonation degree, the amount of ILs precipitation in PLA composites significantly decreased. The precipitation rate of the PLA composite with IL-HSNFC is only 24 % of the counterparts with IL-NFC. This work presents an innovative method to improve interface compatibility, providing a new strategy to reduce plasticizer precipitation and broaden the application scope of PLA.