The design of co-organized nanotube systems with controlled curvature radius that are realized by tilt modulation of co-assembled molecules, induced by the strength of non-covalent interactions in aqueous media, remains a significant challenge. Here, we report success in utilizing a hydrogen bond regulation strategy to stimulate molecular tilt for the formation of nanotubes with controlled curvature radius based on the co-assembly of two kinds of achiral cationic building blocks in aqueous solution. Computations and electron microscopy experiments suggest that the nanotube curvature radius drastically decreases as the tilt angle θ of co-assembled molecules increases with an increase of hydrogen bond strength. Interestingly, a slight change in the co-assembled molecular tilt causes a drastic change in the nanotube curvature radius.
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