Due to the need for high-performance and sustainable building materials, the investigation of the determination of fracture toughness of cement paste using new and sustainable materials, such as cellulose nanocrystals (CNCs) is worthwhile. Contrary to other well-known nano-reinforcement particles, such as carbon nanotubes, CNCs are less toxic; therefore, they have less safety and environmental risks. Fracture behavior of cement paste has been studied intensively for a long time. However, the incorporation of new materials in the cement paste, such as cellulose nanocrystal materials (CNCs), has not been fully investigated. In this paper, the fracture behavior, compressive strength, and hydration properties of cement paste reinforced with cellulose nanocrystal particles were studied. At the age of 3, 7, and 28 days, a three-point bending moment test, and a calorimetry and thermogravimetric analysis, scanning electron microscopy (SEM), and energy dispersive x-ray spectroscopy (EDX) analysis were performed on the water-to-binder-weight ratio of 0.35 cement paste, containing 0.0%, 0.2%, and 1.0% volume cellulose nanocrystals. Results indicated that the fracture properties and compressive strength were improved for the sample containing 0.2% CNCs. Preliminary results indicate that CNCs can improve the fracture behavior of cementitious materials and can be considered as a renewable and sustainable material in construction.