Cellulose nanocrystals (CNCs) were prepared by acidic hydrolysis of cotton fibers (Whatman #1 filter paper). In our efforts to select conditions in which the hydrolysis media does not install labile protons on the cellulose crystals, a mineral acid other than sulfuric acid (H(2)SO(4)) was used. Furthermore, in our attempts to increase the yields of nanocrystals ultrasonic energy was applied during the hydrolysis reaction. The primary objective was to develop hydrolysis reaction conditions for the optimum and reproducible CNC production. As such, the use of hydrobromic acid (HBr) with the application of sonication as a function of concentration (1.5-4.0 M), temperature (80-100 A degrees C), and time (1-4 h) was examined. Applying sonic energy during the reaction was found to have significant positive effects as far as reproducible high yields are concerned. Overall, the combination of 2.5 M HBr, 100 A degrees C, and 3 h associated with the sonication during the reaction generated the highest nanocrystal yields. In addition to the optimization study three types of surface modifications including TEMPO-mediated oxidation, alkynation, and azidation were used to prepare surface-activated, reactive CNCs. Subsequently, click chemistry was employed for bringing together the modified nanocrystalline materials in a unique regularly packed arrangement demonstrating a degree of molecular control for creating these structures at the nano level.