Theranostic nanoparticles with multifunctional ability have been emerging as a new platform for biomedical applications such as imaging, sensing and drug delivery. Despite gold nanorods (Au NRs) being an excellent nanosource with multifunctional versatility, they have certain limitations in biomedical applications, which include surfactant toxicity, biological stability and controlled drug release kinetics. Herein, we have developed Au NR-doxorubicin conjugates (DOX@PSS-Au NR) with improved drug loading efficiency (55 ± 6%) and minimum CTAB toxicity, by employing Au NRs (4.4 ± 0.5 aspect ratio) coated with poly(sodium 4-styrenesulfonate) (PSS). DOX@PSS-Au NR conjugates exhibited higher biological stability with sustained drug release kinetics at pH 5. The binding events of DOX molecules onto the PSS coated gold nanorods (PSS-Au NRs) were monitored through fluorescence quenching and the longitudinal surface plasmon resonance signals. Furthermore the anti-cancer potential and apoptosis inducing efficiency of DOX@PSS-Au NR conjugates in MCF-7 cells revealed higher therapeutic efficiency than free DOX, as corroborated through morphological assessment and in vitro cytotoxicity assay. In addition, DOX@PSS-Au NR conjugates showed efficient cellular entry and uniform intracellular distribution, suggesting the augmenting effect of chemotherapeutic drugs by Au NRs. Thus DOX@PSS-Au NR conjugates demonstrate significant therapeutic potential, suggesting their potential in anticancer therapy.