Drug-eluting stents (DESs) are widely used in the palliative treatment of many kinds of cancers. However, the covered polymers used in DESs are usually associated with stent migration and acute cholecystitis. Therefore, developing noncovered drug-loading layers on metal stents is of great importance. In this work, Ni-Ti layered double hydroxide (Ni-Ti LDH) films were prepared on the surface of nitinol via hydrothermal treatment, and the LDH films were further modified by poly(styrenesulfonate) (PSS). The anticancer drug doxorubicin could be effectively loaded onto the modified films, and drug release could be smartly controlled by the pH. Besides, the drug absorption amounts of cancer cells cultured on the films could be effectively improved. These results indicate that the PSS-modified LDH film may become a promising drug-loading platform that can be used in the design of DESs.