Synthetic self-assembled systems combine responsiveness and reversibility w
ith the ability to perform chemical tasks such as molecular recognition and
catalysis. An unmet challenge is the construction of polymeric materials t
hat, like nature's tubulin. are simultaneously reversible and capable of us
eful physical tasks. We report here a class of reversibly formed polymers t
hat show covalent-polymer mechanical integrity in solution and in the solid
state. Non-Newtonian. polymeric behavior is observed despite the low molec
ular weight of the individual subunits and the seemingly weak forces holdin
g the assemblies together. These polymers assemble through self-complementa
ry hydrogen bonding and by physical encapsulation of small molecules; accor
dingly, the emergent macroscopic structure and function can be controlled b
y appropriate chemical signals.