Supramolecular interactions rely on non‐covalent forces, such as hydrophobic effects, hydrogen‐bonding, and electrostatic interactions, which govern many intracellular biological pathways. In cellulo supramolecular self‐assembly is mainly based on host–guest interactions, changes in pH, enzymes, and polymerization‐induced self‐assembly to accurately induce various unnatural reactions without disturbing natural biological processes. This process can produce synthetic biocompatible macromolecules to control cell properties and regulate biological functions, such as cell proliferation and differentiation. This Minireview focuses on the latest reports in the field of in cellulo supramolecular self‐assembly and anticipates future advances regarding its activation in response to internal and external stimuli, such as pH changes, reactive oxygen species, and enzymes, as well as external light illumination.

Supramolecular interactions rely on non‐covalent forces, such as hydrophobic effects, hydrogen‐bonding, and electrostatic interactions, which govern many intracellular biological pathways. In cellulo supramolecular self‐assembly is mainly based on host–guest interactions, changes in pH, enzymes, and polymerization‐induced self‐assembly to accurately induce various unnatural reactions without disturbing natural biological processes. This process can produce synthetic biocompatible macromolecules to control cell properties and regulate biological functions, such as cell proliferation and differentiation. This Minireview focuses on the latest reports in the field of in cellulo supramolecular self‐assembly and anticipates future advances regarding its activation in response to internal and external stimuli, such as pH changes, reactive oxygen species, and enzymes, as well as external light illumination.