A novel strategy was utilized to develop a stable probe based on thiolated poly(ethylene glycol) (SH-PEG) and polyacrylic acid (PAA) functionalized gold nanorods (GNRs), following the attachment of an anti-cancer drug, doxorubicin (DOX), to obtain PAA-PEG-GNRs@DOX assemblies. Importantly, the obtained probe as a novel drug-delivery and fluorescent imaging agent for simultaneous imaging of and drug delivery to prostate cancer cells has also been demonstrated. In addition to designing PAA-PEG-GNRs that passively target tumor cells for cancer-fighting drug therapy, GNRs are also regarded as hyperthermia agents for photokilling cancer cells, so that the tumor would be attacked on two fronts simultaneously.