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Enzyme-instructed self-assembly (EISA) as a multistep molecular process for selectively killing cancer cells Bing Xu Department of Chemistry, Brandeis University, 415 South St, Waltham, MA 02453 *[email protected] While molecular-targeted therapeutics, which mostly are based on ligand-receptor interaction or enzyme inhibition, have been a key strategy for developing anticancer therapeutics, recent advances in cancer biology have revealed the great complexity of cancers, such as redundant signaling pathways, adaptive drug resistance, genomic instability, intratumoral heterogeneity, and tumor microenvironment. These insights not only elucidate the limitation of the current cancer therapy that aims to only one or two molecular targets (e.g., enzymes, receptors, or transcription factors), but also underscore an urgent need of new approaches for future cancer therapy. In this talk, we highlight enzyme-instructed self-assembly (EISA)—the integration of enzymatic transformation (ET) and self-assembly (SA)--for the development of molecular medicines for future cancer therapy. Enzymatic transformation allows one to develop approaches to target “undruggable” targets or “untargetable” features of cancer cells; self-assembly provides the opportunity for simultaneously interacting with multiple targets. Using the phosphatase catalysis and the self-assembly of small peptides as examples, we will discuss the integration of ET and SA to inhibit multidrug resistance (MDR) cancers in vitro and in vivo, and illustrate a new approach for developing anticancer nanomedicines for targeting multiple hallmarks of cancer that are the major challenges in current cancer therapy.