A multifunctional, dual-drug carrier platform was successfully constructed. Core-shell structured NaGdF₄: Yb/Er@NaGdF₄: Yb@mSiO₂-polyethylene glycol (abbreviated as UCNPS) nanoparticles loaded with the antitumor drug, doxorubicin (DOX) were incorporated into poly(ε-caprolactone) (PCL) and gelatin loaded with antiphlogistic drug, indomethacin (MC) to form nanofibrous fabrics (labeled as MC/UCNPS/DOX) via electrospinning process. The resultant multifunctional spinning pieces can be surgically implanted directly at the tumor site of mice as an orthotopic chemotherapy by controlled-release DOX from mesoporous silicon dioxide (SiO₂) and upconversion fluorescence/magnetic resonance dual-model imaging through NaGdF₄: Yb/Er@NaGdF₄: Yb embedded in MC/UCNPS/DOX in vivo.