The formation of supramolecular polymeric aggregates with a molecular mass of 100 kDa in a nonaqueous solution from a telechelic dimer of isopropylidene guanosine in the presence of K+ ions is reported. The possible structure of macromonomers resulting from the development of G(4) quartets was deduced from DOSY NMR, circular dichroism spectra, and dynamic light scattering measurements. The formation of supramolecular polymeric aggregates with a molecular mass of 100 kDa in a nonaqueous solution from a telechelic dimer of isopropylidene guanosine in the presence of K+ ions is reported. The possible structure of macromonomers resulting from the development of G(4) quartets was deduced from DOSY NMR, circular dichroism spectra, and dynamic light scattering measurements.