To understand the role of electrostatic interactions and hydrogen bonds in the formation of wormlike micelles with the aid of sodium salicylate, two quaternary ammonium surfactants with the headgroup decorated by one hydroxyethyl group N-cetyl-N-(2-hydroxyethyl)dimethylammonium bromide and two hydroxyethyl groups N-cetyl-N,N-di(2-hydroxyethyl)methylammonium bromide, abbreviated as CHEMAB and CDHAB, respectively, were synthesized in this work. Single crystal X-ray diffraction was used to study the intermolecular interactions of surfactants, and (1)H NMR and rheological measurements were employed to investigate the molecular arrangement and morphology of the wormlike micelles. The synergistic interactions of hydrogen bonding and more effective shielding of electrostatic repulsion contribute to the formation and viscoelastic behavior of wormlike micelles. The results also revealed the aggregation behavior of surfactants with hydroxyethyl headgroups in aqueous solutions.