The development of triggered release systems for delivery of peptides and proteins is critical to the success of biological drug therapies. In this paper we describe a dynamic supramolecular system able to capture and release proteins in response to light. The ternary system self-assembles in a dilute aqueous solution of three components: vesicles of amphiphilic cyclodextrin host, noncovalent cross-linkers with an azobenzene and a carbohydrate moiety, and lectins. The cross-linkers form inclusion complexes with the host vesicles, provided the azobenzene is in the trans state. The formation of a ternary complex with lectins requires a high density of cross-linkers on the surface of vesicles. The key innovation in this system is a photoinduced switch from a multivalent, high-affinity state that captures protein to a monovalent, low-affinity state that releases protein. By using isothermal titration calorimetry, dynamic light scattering, UV/vis spectroscopy, and cryogenic transmission electron microscopy, we demonstrate that photoinduced capture and release of lectins in dense multilamellar complexes is highly efficient, highly selective, and fully reversible.