Abstract The use of small organic molecules as catalysts for a wide range of asymmetric transformations has blossomed into a remarkably diverse field under the global heading of organocatalysis. A key central theme of organocatalysis is molecular recognition, which relies on established patterns of reactivity and interactions common to traditional “supramolecular chemistry” such as hydrogen bonding, π‐stacking, cation–π, ionic, and hydrophobic interactions. This chapter presents selected highlights of these approaches in organocatalysis and also compares the way in which Nature's enzymatic supramolecular catalysts have inspired synthetic strategies and modes of action of many organocatalytic approaches to chemical reactivity.