Hydrogel materials have many excellent properties and a wide range of applications. Recently, a new type of hydrogel has emerged: cellulose nanofiber (CNF)-based hydrogels, which have three-dimensional nanofiber networks and unique physical properties. Because CNFs are abundant, renewable, and biodegradable, they are green and eco-friendly nanoscale building blocks. In addition, CNF-based hydrogel materials exhibit excellent mechanical properties and designable functions by different preparation methods and structure designs, demonstrating huge development potential. In this Perspective, we summarize the recent progress in the development of CNF-based hydrogels and introduce their applications in elastic hydrogels, ionic conduction, water purification, and biomedicine, highlighting future trends and opportunities for the further development of CNF-based hydrogels as emerging materials systems.