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Intravascular brachytherapy requires advances in radio‐embolization technologies that combine brilliant radiostability efficacy with a facile and green synthesis route. A hybrid‐integrated radioactive microsphere strategy using phosphorylcholine‐modified lutetium‐177 coordinated polymeric microspheres (177Lu‐PCMs) is reported that are fabricated via radiation‐induced graft polymerization for imaging‐guided...