Abstract：With the vigorous development of the Internet of Things (IoT) and artificial intelligence, the active sensing system based on triboelectric nanogenerators plays an excellent performance potential and application value as a pioneering technology for smart manufacturing. Nevertheless, achieving material innovation to strike a good balance between active sensing systems and environmental friendliness remains a difficult task. As the most abundant biopolymer on earth, the sustainability potential and excellent performance of cellulose are of great importance for the development of smart sensing systems. This review intends to provide a new perspective on the sustainability of smart active sensing systems to design and fabricate cellulosic triboelectric materials for self-powered sensing systems. Herein, the structure and advantageous properties of cellulosic triboelectric materials are briefly described. Furthermore, the structure-property-application relationship of the materials is addressed from the perspective of material design and structure optimization. Next, the latest applications of cellulose triboelectric materials are comprehensively described in smart sensing fields such as environmental monitoring, smart home, smart medical, human-machine interaction, and the Internet of everything. Lastly, the current challenges and future developments of cellulose triboelectric materials for smart sensor systems are presented.