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Ardevines, S.; Marqués-López, E.; Herrera, R. P. Increasing Complexity: Enantioselective Multicatalyzed Multistep Reactions in Enantioselective Organocatalysis: Catalysts, Reactions, and Applications (Ed. Dalko, P.) Wiley-VCH; 2026, 1169–1200. Print ISBN:9783527353408, Online ISBN:9783527845552, DOI:10.1002/9783527845552.

Summary. This chapter presents an overview of enantioselective multicatalyzed multistep reactions as a powerful approach in modern synthetic chemistry. It focuses on the synergistic use of multiple catalysts, particularly combinations of two organocatalysts or an organocatalyst with either transition metal complexes or biocatalysts, to achieve high efficiency, selectivity, and stereocontrol in the synthesis of complex chiral architectures. Inspired by nature’s enzymatic strategies, these cascade and one-pot processes enable efficient access to structurally sophisticated molecules. Special emphasis is placed on organomulticatalysis, with detailed discussion of cooperative, relay, and sequential mechanisms. Pioneering examples illustrate the challenges and opportunities of integrating organocatalysis with biocatalysis or metal catalysis, as well as the use of distinct organocatalysts in tandem. Recent advances in asymmetric cascade reactions and one-pot methodologies are highlighted, revealing their practical relevance and contribution to enhancing molecular complexity, atom economy, and synthetic efficiency.