Cellulose nanocrystals (CNCs) were successfully isolated from oil palm fronds (OPFs) using different concentrations of ammonium persulfate (APS), and their characteristics were analyzed by Fourier transform infrared spectroscopy (FTIR), transmission electron microscopy (TEM), X-ray diffraction (XRD) analysis, and thermogravimetric analysis (TGA). APS oxidation effectively isolated CNCs with rod-like morphology in nanometer scale. The dimensions of the CNCs decreased with increasing APS concentration. FTIR and XRD analyses revealed that all the CNCs showed crystals in the form of cellulose I without crystal transformation occurring during APS treatment. The relative crystallinity of the CNCs increased with increasing APS concentration, whereas their thermal stability decreased. An APS concentration of 2 M was found to be optimal for isolating the CNCs.