For many years, fluorosis has been known as a worldwide disease which seriously diminishes quality of life through skeletal embrittlement and hepatic damage. Aiming to develop novel drugs for simultaneous fluorosis diagnosis and therapy, in this work we explore the feasibility of a novel pyrogallic acid-titanium(iv) complex-modified upconversion nanoprobe (UCNP-PA-Ti) for F- capture and real-time quantification. Utilizing the strong interaction between Ti4+ and F-, the modified PA-Ti decomposes in F--containing solution, which not only weakens the FRET but results in upconversion luminescence (UCL) recovery. Both in vitro and in vivo experiments demonstrate a highly sensitive F- UCL response and therapeutic efficiency, which was promising for successful UCL image monitoring and the therapeutic process. Long blood circulation time and low toxicity ensured their safe application for fluorosis theranostics. Our work provides a new possibility for F- concentration detection within fluorosis therapeutic periods and encourages the development of novel drugs for fluorosis theranostics.