AbstractThe preparation of nanocellulose fibers (NFs) is achieved through pretreating cellulose in a NaOH/urea/thiourea solution, and then defibrillating the fibers through ultrasonication, resulting in a high yield of 85.4%. Extensive work has been done to optimize the preparation parameters. The obtained NFs are about 30 nm in diameter with cellulose II crystal structure. They possess high thermal stability with an onset of thermal degradation at 270 °C and a maximum degradation temperature of 370 °C. Such NFs have potential applications in transistors and batteries with high thermal stability. NFs-H were obtained by homogenizing undefibrillated fibers separated from the preparation of NFs. NFs-H were also in cellulose II crystal form but with lower thermal stability due to low crystallinity. They can be applied to make highly transparent paper.