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The modification of metallodrugs with polyethylene glycol (PEGylation) prolongs blood circulation and improves drug accumulation in tumors; it represents a general strategy for drug delivery. However, PEGylation hinders cellular internalization and tumor penetration, which reduce therapeutic efficacy. Herein, the red\u2010light\u2010enhanced cellular internalization and tumor penetration of a PEGylated anticancer agent, PEGylated Ru complex (Ru\u2010PEG), are reported upon. Ru\u2010PEG contains a red\u2010light\u2010cleavable PEG ligand, anticancer Ru complex moiety, and fluorescent pyrene group for imaging and self\u2010assembly. Ru\u2010PEG self\u2010assembles into vesicles that circulate in the bloodstream and accumulate in the tumors. Red\u2010light irradiation induces dePEGylation and changes the Ru\u2010PEG vesicles to large compound micelles with smaller diameters and higher zeta potentials, which enhance tumor penetration and cellular internalization. Red\u2010light irradiation also generates intracellular <jats:sup>1<\/jats:sup>O<jats:sub>2<\/jats:sub>, which induces the death of cancer cells. This work presents a new strategy to enhance the cellular internalization and tumor penetration of anticancer agents for efficient phototherapy.<\/jats:p>","DOI":"10.1002\/smll.202205461","type":"journal-article","created":{"date-parts":[[2022,11,11]],"date-time":"2022-11-11T08:21:37Z","timestamp":1668154897000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":33,"title":["Amphiphilic Metallodrug Assemblies with Red\u2010Light\u2010Enhanced Cellular Internalization and Tumor Penetration for Anticancer Phototherapy"],"prefix":"10.1002","volume":"18","author":[{"given":"Xiaolong","family":"Zeng","sequence":"first","affiliation":[{"name":"CAS Key Laboratory of Soft Matter Chemistry Anhui Key Laboratory of Optoelectronic Science and Technology Department of Polymer Science and Engineering University of Science and Technology of China  Hefei 230026 China"},{"name":"Max Planck Institute for Polymer Research  Ackermannweg 10 55128 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