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This invention relates to a method for regulating zirconium-based metal-organic framework nanoparticles using carboxylated cellulose nanoparticles. This method utilizes carboxylated cellulose nanoparticles, a green and environmentally friendly material, as a defect modulator, and obtains UiO-66-OH with tunable defect levels via an in-situ one-pot synthesis. Using carboxylated nanoparticles as a nano-soft template, carboxyl competitive ligands, and surface-assisted growth medium, the method induces the heterogeneous nucleation and explosive growth of UiO-66-OH crystals into nanospheres. Precise defect regulation is achieved through the precise competitive coordination of carboxyl groups and zirconium ions. While achieving defect regulation and ensuring stability, background fluorescence is modulated through the disruption of intramolecular charge transfer (ICT). This provides a solid research foundation for the regulation of defective metal-organic framework materials and their bio-friendly applications.