Combination therapy with different functional drugs has been proved to be an effective strategy for cancer treatments by achieving cooperative therapeutic efficacy and reducing drug side effects. In this study, a novel combination anticancer system was designed by coating silver nanoparticles in the poly(aspartic acid) (PAsp) shell of polymer micelle via the in situ reduction of silver ions and encapsulating doxorubicin (DOX) into the micellar poly(ε-caprolactone) (PCL) core through hydrophobic interaction. This combination system not only avoided aggregation of the silver nanoparticles but also improved the bioavailability of DOX. As a result, it exhibited enhanced antitumor activity against HepG2 tumor cells compared with single silver-coated or DOX-loaded nanoparticles because of the combined anticancer effects of nanosilver and DOX. Therefore, this combination therapeutic system could be a potential candidate for enhanced anticancer therapy.