Cellulose has received a tremendous amount of attention both in academia and industry owing to its unique structural features, impressive physical–chemical properties, and wide applications. This natural polymer is originally used for packaging, paper, lightweight composites, and so forth and is now being developed for various new areas, such as antibacterial treatment, catalysis, water purification and separation, and biological and environmental analysis. In the current article, we summarize the recent developments in the self-assembly of cellulose with various species including metal ions and metal and metal oxide nanoparticles. Then we highlight several key application areas of cellulose-based composites by reviewing the recent representative literature in each area. A significant part of this review demonstrates some exciting innovations for a wide range of practical applications of cellulose-based composites. Some challenges are also discussed with a view toward future developments.