Cation-controlled assembly, activity, and organisation of biomimetic DNA receptors in synthetic cell membranes

Biological cells use cations as signalling messengers to regulate a variety of responses. Linking cations to the functionality of synthetic membranes is thus crucial to engineering advanced biomimetic agents, such as synthetic cells. Here, we introduce bio-inspired DNA-based receptors that exploit non-canonical G-quadruplexes for cation-actuated structural and functional responses in synthetic lipid membranes. Membrane confinement grants cationdependent control over receptor assembly and, when supplemented with hemin co-factors, their peroxidase DNAzyme activity. Cationmediated control extends to receptor lateral distribution to localise DNA-based catalysis within phase-separated membrane domains of model synthetic cells, imitating the localisation of multimeric membrane complexes to signalling hubs in living cells. Our modular strategy paves the way for engineering from the bottom-up cation-responsive pathways for sensing, signalling, and communication in synthetic cellular systems.