Probing the Structure and Mechanics of Intertwined Homo- and Hetero-Supramolecular Gel Noodles

Shaping supramolecular hydrogels formed using low molecular weight gelators (LMWGs) into architecturally complex and multifunctional materials is a significant challenge. Here, we introduce a strategy to mechanically twist multiple 1D supramolecular gel filaments (gel noodles) into robust, multifunctional, and stimuli-responsive structures. Twisting introduced mechanical interlocking, which in two identical filaments yielded marginal improvement in tensile performance, while compositionally distinct gel noodles exhibited up to ~25% increase in strength due to effective load redistribution and frictional contact. However, twisting three or more filaments reduced mechanical strength, likely due to high internal strain and the formation of misaligned bundles—an effect consistent with stochastic failure propagation in twisted fibre assemblies. These results highlight the dual nature of intertwining multiple noodles: it can reinforce or compromise mechanical robustness depending on geometry and filament interactions. Despite this, twisting chemically distinct noodles enabled the formation of robust structures with spatially separated functionalities, such as photoresponsiveness, while maintaining structural integrity. This modular strategy offers a tunable platform for engineering hierarchical materials suited for soft robotics, adaptive scaffolds, and responsive delivery systems.