AbstractThere is currently considerable interest in developing stiff, strong, tough, and heat resistant poly(lactide) (PLA) based materials with improved melt elasticity in response to the increasing demand for sustainable plastics. However, simultaneous optimization of stiffness, strength, and toughness is a challenge for any material, and commercial PLA is well‐known to be inherently brittle and temperature‐sensitive and to show poor melt elasticity. In this study, we report that high‐shear mixing with cellulose nanocrystals (CNC) leads to significant improvements in the toughness, heat resistance, and melt elasticity of PLA while further enhancing its already outstanding room temperature stiffness and strength. This is evidenced by (i) one‐fold increase in the elastic modulus (6.48 GPa), (ii) 43% increase in the tensile strength (87.1 MPa), (iii) one‐fold increase in the strain at break (∼6%), (iv) two‐fold increase in the impact strength (44.2 kJ/m2), (v) 113‐fold increase in the storage modulus at 90°C (787.8 MPa), and (vi) 103‐fold increase in the melt elasticity at 190°C and 1 rad/s (∼105 Pa) via the addition of 30 wt% CNC. It is hence possible to produce industrially viable, stiff, strong, tough, and heat resistant green materials with improved melt elasticity through high‐shear mixing.