A small library of dendrimers based on triazines was prepared by varying the surface and interior linking groups to study the relationship between structure and the ability of some of these dendrimers to gel in acidified organic solvents including chloroform, methylene chloride, and benzene. Convergent, divergent, and semiconvergent routes yielded eight molecules comprising p-aminobenzylamine or piperazine linking groups and piperidine or butylamine surface groups. Dendrimers that incorporate interior and surface groups capable of hydrogen bonding (p-aminobenzylamine or butylamine) gel at lower concentrations than those groups that offer no hydrogen-bonding protons (piperazine or piperidine). In some cases, these latter molecules do not form gels to the limit of solubility. Studies with competitive solvents corroborate hydrogen bonding, but neither IR nor NMR spectroscopy reveals signals that substantiate this hypothesis. TEM studies show fibers. Studies of these systems at concentrations below that required for gelation indicate the presence of aggregates in solution: an assay using gel permeation chromatography offers predictive ability for gelation.