The coupling of diagnostic capability and effective therapy in a single multifunctional nanomedicine is desirable but remains challenging. Here, we developed multifunctional nanoparticles consisting of a gold nanostar (AuNS) core with a shell of metal-drug coordination polymer (CP). The AuNS core enabled plasmonic photothermal effect and two-photon photoluminescence (TPL), while the CP shell of gadolinium and gemcitabine monophosphate allowed chemotherapy and MRI imaging. The AuNS@CP nanoparticles exhibited a strong T1 contrast signal and could monitor the localization of nanoparticles in vivo through noninvasive MR imaging, while intravital TPL imaging could be used to study nanoparticle behavior in tumors at the microscopic level. The combination of photothermal therapy and chemotherapy inhibited tumor growth in vivo