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The use of self-assembled nanostructures consisting of red-light-responsive Ru(II)-containing block copolymers (BCPs) for anticancer phototherapy is demonstrated. Three Ru-containing BCPs with different molecular weights are synthesized. Each BCP contains a hydrophilic poly(ethylene glycol) block and an Ru-containing block. In the Ru-containing block, more than half of the side chains are coordinated with [Ru(2,2′:6′,2′′-terpyridine)(2,2′-biquinoline)]2+, resulting in more than 40 wt% Ru complex in the BCPs. The Ru complex acts as both a red-light-cleavable moiety and a photoactivated prodrug. Depending on their molecular weights, the BCPs assemble into micelles, vesicles, and large compound micelles. All of the BCP assemblies are taken up by cancer cells. Red-light irradiation releases the Ru complex and generates singlet oxygen (1O2) in cancer cells. The released Ru complex and 1O2 inhibit the growth of cancer cells. Among the three BCP assemblies, the BCP micelle exhibits the most efficient cellular uptake and best anticancer performance.Self-assembled nanostructures of red-light-responsive Ru(II)-containing block copolymers are used for anticancer photo-therapy. The Ru complexes in the block copolymers are photocleavable and anticancer agents. Red light releases the Ru complexes and generates singlet oxygen in cancer cells. A moderate irradiation dose, which prevents photodamage, is sufficient to inhibit the growth of cancer cells.