Boosting the Strength and Toughness of Polymer Blends via Ligand‐Modulated MOFs

Abstract Mechanically robust and tough polymeric materials are in high demand for applications ranging from flexible electronics to aerospace. However, achieving both high toughness and strength in polymers remains a significant challenge due to their inherently contradictory nature. Here, a universal strategy for enhancing the toughness and strength of polymer blends using ligand‐modulated metal–organic framework (MOF) nanoparticles is presented, which are engineered to have adjustable hydrophilicity and lipophilicity by varying the types and ratios of ligands. Molecular dynamics (MD) simulations demonstrate that these nanoparticles can effectively regulate the interfaces between chemically distinct polymers based on their amphiphilicity. Remarkably, a mere 0.1 wt.% of MOF nanoparticles with optimized amphiphilicity (ML‐MOF (5:5) ) delivered ≈1.1‐ and ≈34.1‐fold increase in strength and toughness of poly (lactic acid) (PLA)/poly (butylene succinate) (PBS) blend, respectively. Moreover, these amphiphilicity‐tailorable MOF nanoparticles universally enhance the mechanical properties of various polymer blends, such as polypropylene (PP)/polyethylene (PE), PP/polystyrene (PS), PLA/poly (butylene adipate‐co‐terephthalate) (PBAT), and PLA/polycaprolactone (PCL)/PBS. This simple universal method offers significant potential for strengthening and toughening various polymer blends.