The multifunctional theranostic nanoplatform based on the combination of persistent luminescent nanoparticles (PLNPs) and metal-organic frameworks (MOFs) has both in vivo imaging and tumor therapeutic drug-loading functions, providing a new strategy for accurate and effective tumor diagnosis and treatment. Herein, the near-infrared (NIR) PLNP SiO2@Zn1.05Ga1.9O4:Cr was combined with HKUST-1 MOFs to form a core-shell structure theranostic nanoplatform which possessed the triple function of autofluorescence-free NIR PersL bioimaging, tumor chemodynamic therapy (CDT), and tumor photothermal therapy (PTT). Also, the photothermal conversion efficiency reached 58.7%, which is superior to the reported nano metal-organic framework (NMOF) photothermal reagents. We demonstrated that the nanoplatform could enter the tumors of mice within 0.5 h and could be target-activated by H2O2 and H2S in the tumor cells, resulting in effective PTT and CDT synergistic treatment. Tumor-bearing mice experiments showed that the tumor could be completely cured without harming normal tissue. This theranostic nanoplatform may provide a promising strategy showing imaging, PTT, and CDT synergistic treatment tri-mode for clinical cancer therapy.