A facile method is reported to prepare nanocellulose fibers from oil palm trunk fibers. The fibers were pretreated 2 hours with NaOH/urea solution, and the fully swelled fibers were mechanically treated through high-pressure homogenization to obtain nanocellulose. The nanocellulose fibers were characterized by Fourier transform infrared spectroscopy (FTIR), X-ray diffraction analysis (XRD), thermogravimetric analysis (TGA), and scanning electron microscopy (SEM). FTIR results revealed that there was no obvious difference between the spectra of the bleached fibers (BF), pretreated cellulose fibers (PCF), and cellulose nanofibers (NCF), which indicated that the pretreatment process is a non-derivative reaction. The crystallinity of PCF and NCF decreased and contained the cellulose I crystal structure. The PCF presented both a distorted structure and a coarser surface. The resulting NCF were approximately 10 nm to 100 nm in diameter with the length varying from hundreds of nanometers to several micrometers, as observed by SEM. The thermal degradation of NCF was 223 °C with about 20% weight loss, and the maximum degradation temperature was 338 °C. NaOH/urea showed potential as a mild solvent for preparing nanocellulose fibers.