Designing
of supramolecular hydro-/organogels having desired properties,
biocompatibility, and stimuli responsiveness is a challenging task.
Herein, the gelation ability of amphiphilic glycolipid-based gelators
in a wide range of solvents is explored. The structure–function
relationship was established by varying the chain length and polar
headgroup size of amphiphilic gelators. The prepared hydro-/organogels
were characterized by employing several techniques such as differential
scanning calorimetry (DSC), rheology, field emission scanning electron
microscopy (FE-SEM), high-resolution transmission electron microscopy
(HR-TEM), X-ray diffraction (XRD), etc. The thermal stability of hydro-/organogels
increased with an increase in chain length. Rheological analysis depicted
that variation in chain length and headgroup size of amphiphilic gelators
significantly affected the gel strength and stability. The self-assembled
morphology of hydro-/organogel samples revealed the compact entangled
fibrillar network structures. After comparing the energy-minimized
molecular length with the d-spacing value obtained
by XRD, interdigitated bilayer packing in the gel network was established.
The bioactive encapsulation and enzymatic release study of hydro-/organogels
portrayed their potential application in the biomedical field. To
our delight, glycolipid 16M (C16 chain length) formed
a molecular hydrogel with injectable and thixotropic behaviors. High
critical strain value, thixotropy, injectability, thermoreversibility,
and faster bioactive release for the 16M-W hydrogel proved
crucial to predict its future applications. Overall, glycolipid amphiphiles
designed by upholding proper hydrophilic–lipophilic balance
can form multifunctional supramolecular hydrogels with excellent implementation
in the drug delivery system.