Recently, smart labels for monitoring food freshness provided a powerful strategy to reduce food waste and foodborne diseases. Excellent performance, non-toxicity, and simple process were great challenges for large-scale production of smart labels. The present study proposed a one-pot approach of green preparation for smart labels integrated with curcumin/starch nanoparticles/natural deep eutectic solvents self-assembly system. The curcumin-loaded starch nanoparticles significantly improved the mechanical properties, water resistance and UV resistance of smart labels. The sensitivity to volatile amines was improved, resulting from an increase in the dispersibility of curcumin. In addition, during the monitor of shrimp freshness, the total volatile salt-based nitrogen in shrimp reached 13.23 mg/100 g after 18 h of storage, concomitant with a significant shift in the color of smart labels from yellow to orange. These results highlight the self-assembly system could be directly exploited as readily manufacturable modules to develop a simple industrial method for smart labels.