We report on the assembly of gold nanorods functionalized with poly(ethylene glycol) in aqueous suspensions by electrostatic control and hydrogen bonds provided by polyelectrolyte linkers (i.e., interpolymer complexation processes). Small-angle X-ray scattering reveals that the quality and stability of the assemblies into the hexagonal columnar phases increase with temperature. Our study shows that the lattice constant of the ordered structures is tunable over a wide range of values by the interplay between electrostatic and hydrophobic effects.