Cellulose nanocrystal (CNC) is a promising sustainable material with its biocompatibility, high aspect ratio, and mechanical strength. CNC-based systems have potential applications in various fields including biosensors, packaging, coating, energy storage, and pharmaceuticals. However, turning CNC into smart systems remains a challenge due to the lack of stimuli-responsiveness, limitation in compatibility with hydrophobic matrices, and their agglomeration tendency. In this work, a thermo-responsive nanocomposite system is constructed with CNCs and polymersome forming Pluronic L121 (L121), and its phase behavior and mechanical properties are investigated in detail. Two different CNC concentration (4 % and 5 %) is studied by changing the L121 concentration (1–20 %) to understand the effect of unimers and polymersomes on the CNC network. At dilute L121 concentrations (1–5 %), the composite system becomes softer but more fragile below the transition temperature. However, it becomes much stronger at higher L121 concentrations (10–20 %), and a gel network is obtained above the transition temperature. Interestingly, the elastically reinforced CNC gels exhibit greater resistance to microstructural breakdown at large strains due to the soft and deformable nature of the large polymersomes. It is also found that the gelation temperature for hydrogels is tunable with increasing L121 concentration, and the nanocomposite hydrogels displayed thermo-reversible rheological behavior.