The relationship between chemical structure and gelation ability was examined for a series of nine Hg-containing compounds. Both solid-state properties (dissolution enthalpies/entropies and packing structure) and gel properties (strength, morphology, cation selectivity, and anion tolerance) were examined. Overall, the results reveal a complex relationship between chemical structure and properties. The remediation potential of these Hg-triggered gelations was also investigated, revealing that >98% of the Hg2+ in water can be removed through gel formation.