Recently, paper substrates have attracted tremendous interest from both academia and industry. Not only is paper highly abundant and portable, it is lightweight, disposable, easy-to-use, and can be rolled or folded into 3D configurations. More importantly, with a unique porous bulk structure and rough and absorptive surface properties, the construction of nanomaterials-functionalized cellulose has enabled cellulose paper to be applied for point-of-care (POC) paper devices with reasonably good performance at low cost. In this review, the latest advances in the modification of nanomaterials on paper cellulose are summed up. To begin with, the attractive properties of paper-based analytical devices are described. Then, fabricating methods for the functionalization of cellulose with diverse materials, including noble metals, bimetals, metal oxides, carbon nanomaterials, and molecular imprinting polymer nanoparticles, as well as their applications, are introduced in detail. Finally, the current critical issues, challenges, and future prospectives for exploring a paper-based analytical system based on nanomaterials-modified cellulose are discussed. It is believed that more strategies will be developed in the future to construct nanomaterials-functionalized cellulose, paving the way for the mass production of POC paper devices with a satisfactory performance.