The present disclosure discloses methods and compositions for A administering Cerenkov radiation-induced therapy (GRIT). In an aspect, the invention encompasses a composition comprising at least two radiation-sensitive molecules. In another aspect, the invention encompasses a composition comprising a radiation-sensitive molecule and a targeting agent. In still another aspect, the invention encompasses a method for administering Gerenkov radiation-induced therapy (GRIT) to a target tissue in a subject. The method comprises administering to the subject an effective amount of a composition B comprising at least one radiation-sensitive molecule and administering to the subject an amount of a Gerenkov radiation (GR)-emitting radionuclide effective to activate the radiation-sensitive molecule, thereby administering GRIT to the target tissue in the subject.