In this study, the fingerprint of the acid concentration during the hydrolysis process on the optical band gap of cellulose nanocrystals (CNCs) has been systematically studied. The CNCs have been prepared using hydrochloric acid at a hydrolysis temperature of 50°C and at a constant hydrolysis time of 4 hours but with varying hydrochloric acid concentrations of 5%, 10% and 15%. The crystalline structure and phase identification of the CNCs have been studied using XRD technique. UV-Vis Spectroscopy has been done and the optical band gap energy calculated by performing the Tauc’s plot. From the study, the grain size has been found to decrease with acid concentration while the band gap energy has been found to increase with increasing acid concentration. Further, the optical band gaps of the CNCs have been found to decrease with the increase in crystallite size. This shrinkage of the band gap has been attributed to the increased impurity concentration leading to the narrowing of the band gap due to the emerging of the impurity band formed by the overlapped impurity states.