ABSTRACTCellulose nanocrystals (CNC) are isolated from office waste paper using an alkali solution and a subsequent acid hydrolysis process. The Fourier transform infrared spectroscopy and X‐ray diffraction (XRD) results demonstrate that ink and fillers used in the papermaking industry are almost totally removed after alkali treatments. The XRD results show that CNCs obtained after 2 wt % NaOH solution treatment and a subsequent hydrolysis process exhibit only a cellulose I crystalline structure, and the crystallinity index value increases around 42% with respect to initial office waste paper. Nevertheless, CNCs obtained after 7.5 wt % NaOH solution treatment and a subsequent acid hydrolysis process show a mixture of cellulose I and cellulose II polymorphs. The thermal analysis shows that the CNCs obtained after 7.5 wt % NaOH solution treatment and a subsequent acid hydrolysis process are thermally less stable than other samples, suggesting that the cellulose chains could depolymerize into low molecular weight sugar compounds. Even though the atomic force microscopy images confirm the presence of CNCs, the optical images show that some cellulose microfibers still maintain their structure. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017, 134, 45257.