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A facile strategy to fabricate gold nanorod@polyacrylic acid/calcium phosphate (AuNR@-PAA/CaP)yolk–shell nanoparticles(NPs)composed with a PAA/CaP shell and an AuNR yolk is reported. The as-obtained AuNR@PAA/CaP yolk–shell NPs possess ultra-high doxorubicin (DOX) loading capability (1 mg DOX/mg NPs),superior photothermal conversion property(26%) and pH/near-infrared (NIR) dual-responsive drug delivery performance. The released DOX continuously increased due to the damage of the CaP shell at low pH values.When the DOX-loaded AuNR@PAA/CaP yolk–shell NPs were exposed to NIR irradiation,a burst-like drug release occurs owing to the heat produced by the AuNRs. Furthermore, AuNR@PAA/CaP yolk–shell NPs are successfully employed for synergic dual-mode X-ray computed tomography/photoacoustic imaging and chemo-photother-mal cancer therapy. Therefore, this work brings new insights for the synthesis of multifunctional nanomaterials and extends theranostic applications.