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Harnessing noncovalent interactions to create controlled routes to functional materials with nanoscopic dimensions is a key challenge in contemporary chemical science. The use of molecular species, polymers, and nanoparticles as building blocks combined with self-assembly approaches that involve hydrogen-bonding, π-stacking, coordination or metallophilic interactions (1–5), immiscibility and solvophobicity (6–8), or crystallization (9) has led to a range of important recent advances. The introduction of further complexity through multistep processing and the manipulation of the resulting nanostructures through attenuation and enhancement of noncovalent forces represent examples of important further goals, but much remains to be achieved with respect to these objectives. On page 499 of this issue, Fukino et al. (10) provide an elegant demonstration of how π-stacking and metallophilic interactions can be used to control the assembly of ferrocene-based molecular building blocks into ordered and complex nanoscale objects. They report the selective assembly of ferrocene-based units into large-diameter nanotubes that can then be reversibly cleaved into nanorings.