Synthetic supramolecular polymers, composed of monomers that self-assemble in solution via reversible, non-covalent interactions, are important platforms for the development of advanced materials for many applications. Such polymers are formed by monomeric units interacting via hydrogen bonding, solvophobic repulsion, π-π stacking, etc. Thanks to such reversible interactions, supramolecular polymers bear unique dynamical properties at the equilibrium, which are at the basis of stimuli-responsive and adaptive features reminiscent of living materials. While, in principle, changing the monomer structure allows tuning the dynamic properties of supramolecular polymers, the complexity of these systems makes it often impossible to obtain clear monomer-assembly relationships. Various experimental approaches were used to characterize the structure of supramolecular polymers in solution, most often providing average information on the entire solution, with limited detail on the distribution of aggregate sizes. Considerable efforts were spent also in characterizing the dynamics of supramolecular polymers using, e.g., Förster Resonance Energy Transfer (FRET), Stochastic Optical Reconstruction Microscopy (STORM), or Hydrogen/deuterium exchange (HDX) mass spectrometry. Typically, such approaches allow studying supramolecular polymer dynamics at the level of statistical ensembles or of individual assemblies (e.g., using bulky labeling groups, STORM detects supramolecular exchange with a resolution of ∼ 20-50 nm). However, obtaining a clear understanding of the molecular processes that, in concert, define the dynamic nature of supramolecular polymers would ideally require a complete characterization of such systems with submolecular resolution, which is mostly inaccessible via experiments.