AbstractBio‐inspired approaches in materials science and systems chemistry are yielding a variety of stimuli‐responsive and dynamic materials that are gradually changing our everyday life. However, the ability to chemically program these materials to exhibit macroscopic higher‐order behaviours such as self‐assembly, contractility, swarming, taxis, chemical communication, or predator‐prey dynamics remains an ongoing challenge. While still in its infancy, the successful fabrication of bio‐inspired materials displaying higher‐order behaviours not only will help bridging the gap between living and non‐living matter, but it will also contribute to the development of advanced materials for potential applications ranging from tissue engineering and biotechnology, to soft robotics and regenerative medicine. Our Mini‐Review will systematically discuss the higher‐order behaviours developed thus far in bio‐inspired systems, namely (i) polymer networks (ii) microbots, (iii) protocells, and (iv) prototissues. For each system it will provide key examples and highlight how the emergent behaviour could be chemically programmed.