Oppositely charged surfactants and polyelectrolytes undergo associative phase separation when mixed in near-stoichiometric ratios. In recent years this phenomenon has been exploited to form ordered gel-like assemblies, whose structure ranges from spherical particles (1 – 4000 µm in diameter) to cylindrical fibers and planar sheets. The stability of these materials depends on the equilibrium phase behavior of the surfactant and polyelectrolyte mixture, while their structure is governed by the method of their preparation. Here, we discuss the performance of these materials in controlled release and tissue engineering applications: namely, the encapsulation of aromatic oil (cymene) for fragrance release and cell guidance for regenerative medicine. Surfactant and polyelectrolyte gel particles release aromatic oils into both aqueous and organic receiving solutions, with rates determined by the solubility and diffusivity of the oil in the gel matrix. Likewise, cylindrical surfactant and polyelectrolyte gel fibers prepared from biocompatible components can act as cell-adhesive scaffolds that guide cell growth.