Natural cellulose fiber-based materials have been widely used in daily life for a broad application owing to their intrinsic merits such as easy availability, eco-friendly, good processability, and outstanding physical-mechanical properties. Surface modification of natural fibers with nanostructures is an effective strategy to integrate the textile substrates with many favorable functionalities. Here, a green, facile, and universal method is introduced for the in situ growth of γ-cyclodextrin (γ-CD) metal-organic frameworks (MOFs) in cellulose fiber-based materials (CelluMOFs). Compared to the pristine fibers, the resulting CelluMOFs have high porosity with up to 50 times larger specific surface area and enhanced loading capacity to functional molecules (essential oils, antibacterial agents, and active drugs) with 23-36 times higher loading content. The CelluMOFs also exhibit high adsorption capability to volatile organic compounds and carbon dioxide. Moreover, the CelluMOFs textiles loaded with a model drug (doxorubicin) show a steady release profile and deep skin permeation capability. These CelluMOFs combine the advantages of both cellulose fibers and CD-MOFs, which greatly extend their applications in the fragrance industry, antimicrobial, pollutant removal, and biomedical textiles.