This study investigates the effect of cellulose nanocrystal (CNC) on the mechanical properties of cement/fly ash pastes under various water/binder ratios through a series of tests, including mechanical test, isothermal calorimetry test, X-ray diffraction test, and mercury intrusion porosimetry test. The results indicate that CNCs have a significant enhancing effect on the mechanical properties of cement/fly ash-cement pastes, with this enhancement being influenced by fly ash and water/binder ratio. CNC has an evident promoting influence on the cumulative heat and heat release rate of cement/fly ash-cement pastes. Higher CNC dosage exhibits a faster hydration reaction in cement pastes with 10 % fly ash. Additionally, with an increase in CNC dosage, there is a rise in the hydration product dosage of cement/fly ash-cement pastes, accompanied by an increase in the proportion of gel pores and transition pores. The study provides insights into potential applications of CNC to enhance the mechanical performance of cement/fly ash-based composites in construction industry.