Disulfiram (DSF) exerts potent anticancer activity via the formation of chelates with copper or zinc ions in tumor tissues, but the low abundance of these ions in the tumor cannot sustain its antitumor activity. Herein, we show that a zwitterionic water-soluble N-oxide polymer, poly[2-(N-oxide-N,N-dimethylamino)ethyl methacrylate] (OPDMA), can complex cupric ions and form nanogels (OPDMA/Cu), which efficiently deliver copper ions to tumor tissue to potentiate DSF significantly for effective antitumor therapy.