We systematically investigate model synthetic and natural bottlebrush polyelectrolyte solutions through an array of experimental techniques (osmometry and neutron and dynamic light scattering) along with molecular dynamics simulations to characterize and contrast their structures over a wide range of spatial and time scales. In particular, we perform measurements on solutions of aggrecan and the synthetic bottlebrush polymer, poly(sodium acrylate), and simulations of solutions of highly coarse-grained charged bottlebrush molecules having different degrees of side-branch density and inclusion of an explicit solvent and ion hydration effects. While both systems exhibit a general tendency toward supramolecular organization in solution, bottlebrush poly(sodium acrylate) solutions exhibit a distinctive "polyelectrolyte peak" in their structure factor, but no such peak is observed in aggrecan solutions. This qualitative difference in scattering properties, and thus polyelectrolyte solution organization, is attributed to a concerted effect of the bottlebrush polymer topology and the solvation of the polymer backbone and counterions. The coupling of the polyelectrolyte topological structure with the counterion distribution about the charged polymer molecules along with direct polymer segmental hydration makes their solution organization and properties "tunable," a phenomenon that has significant ramifications for biological function and disease as well as for numerous materials applications.