Herein we demonstrate the design and synthesis of liquid crystalline gels through multi-scale hierarchical self-assembly of LAPONITE® and amidodiol in water. These two components interact with each other through non-covalent interactions, such as hydrogen bonding and ion–dipole interactions, to form highly ordered superstructures in different dimensions and length scales. Effects of concentration of amidodiol and timescale on specific modes of packing were studied using various microscopic and spectroscopic techniques, such as PLM, SEM, TEM, XRD, rheology and FTIR. Presence of hydroxyl groups was confirmed by chemical analysis. A plausible mechanism for the formation of superstructures in functionalized LAPONITE®–amidodiol gel (FLAG) was proposed. Electrochemical impedance studies of the FLAG showed low charge transfer resistance (245 Ω) with a stable rectangular electrochemical window (−0.4 V to 1.5 V). Galvanostatic studies revealed good cycling stability with a specific capacitance of 1856 mF g−1. Results suggest that FLAGs can be exploited as an efficient gel electrolyte in energy storage devices.
