The improvement of high‐Z‐based metallic nanostructures as radiosensitizers with high monolithicity and versatility by superadditive therapeutic track and the good protective effect is considerable, but they are limited by some problems such as nonideal selectivity for the target tissue. In this study, nanosystems were developed to enhance the efficacy of radiotherapy and reduce cancer cell survival based on innovative gold (Au) functionalized oxygen‐single‐walled carbon nanotubes (O‐SWCNTs). We illustrate the use of folic acid (FA) as a targeting agent and bovine serum albumin (BSA) to stabilize the physiological environment and increase durability. The physical and chemical properties of the nanosystems were evaluated using transmission electron microscopy (TEM), selected area electron diffraction (SAED), dynamic light scattering (DLS), zeta potential, X‐ray diffraction (XRD), ultraviolet–visible (UV–Visible), and Fourier transform infrared (FTIR) techniques. Finally, the MTT assay was used to investigate the therapeutic effects of nanoparticles in the 4 T1 mouse breast cancer model in the presence and absence of X‐rays. So, the cancer cells experienced a more effective reduction in survival after receiving O‐SWCNTs‐Au‐BSA‐FA + 8 Gy than O‐SWCNTs‐BSA, Au‐BSA‐FA, and O‐SWCNTs‐Au‐BSA + 8 Gy groups.