The parenchymal cells in bamboo are an attractive source of raw materials due to their low degree of lignification and relatively loose cell wall structures. In this study, nanocellulose fibrils (NCFs) were isolated via a combined process of ultrasonication and chemical pretreatment of parenchymal cells separated from Moso bamboo (Phyllostachys pubescens) by means of a simple screening approach. As indicators of the fibrillation degree served the morphology, optical properties, and dynamic viscosity of the prepared NCF hydrogel as function of ultrasonication time. The mechanical properties of NCF derived films were also determined. The results show that high-quality NCFs can easily be prepared from bamboo parenchymal cells through the above-mentioned process, with an optimal ultrasonication time of 40 min. The utilization of bamboo processing residues via the ultrasonication route is promising and for energy saving production of high-quality NCFs at large scale.