Hypothesis: Multi-component supramolecular hydrogels are gaining increasing interest as stimuli-responsive materials. To fully understand and possibly exploit the potential of such complex systems, the hierarchical structure of the gel network needs in-depth investigations across multiple length scales. We show that a thorough structural and rheological study represents a crucial pillar for the exploitation of this class of functional materials. Experiments: Supramolecular hydrogels are prepared by self-assembly of hexadecyltrimethylammonium bromide (CTAB) and azobenzene-4,40-dicarboxylic acid (AZO) in alkaline aqueous solution. The CTAB/AZO concentration was varied from phi = 0.25 to 4 wt% keeping the CTAB:AZO molar ratio fixed at 2:1. The systems were thoroughly studied through a combination of X-ray scattering, microscopy, rheological and spectroscopic analyses. Findings: The CTAB/AZO solutions form a self-supporting gel with nanofibrillar structure below similar to 30 degrees C. The critical gelation concentration is phi(c) = 0.45 wt%. Above this threshold, the gel elasticity and strength increase with CTAB/AZO content as similar to(phi-phi(c))(1). The hydrogels exhibit self-healing ability when left at rest after a stress-induced damage. Moreover, the light-induced isomerization of the AZO moieties provides the gel with light-responsiveness. Overall, the multi-stimuli responsiveness of the studied CTAB/AZO hydrogels makes them a solid starting point for the development of sensors for mechanical vibrations and UV/visible light exposure. (C) 2020 Elsevier Inc. All rights reserved.