Mechanochromic, Structurally Colored, and Edible Hydrogels Prepared from Hydroxypropyl Cellulose and Gelatin

Hydroxypropyl cellulose (HPC) is an edible, cost‐effective and widely used derivative of cellulose. Under lyotropic conditions in water, HPC forms a photonic, liquid crystalline mesophase with an exceptional mechanochromic response. However, due to insufficient physical cross‐linking photonic HPC can flow freely as a viscous liquid, preventing the exploitation of this mechanochromic material in the absence of any external encapsulation or structural confinement. Here this challenge is addressed by mixing HPC and gelatin in water to form a self‐supporting, viscoelastic, and edible supramolecular photonic hydrogel. It is demonstrated that the structural coloration, mechanochromism and non‐Newtonian shear‐thinning behavior of the lyotropic HPC solutions can all be retained into the gel state. Moreover, the rigidity of the HPC‐gel provides a 69% shorter mechanochromic relaxation time back to its initial color when compared to the liquid HPC–water only system, broadening the dynamic color range of HPC by approximately 2.5× in response to a compressive pressure. Finally, the ability to formulate the HPC‐gels in a scalable fashion from only water and “food‐grade” constituents unlocks a wide range of potential applications, from response‑tunable mechanochromic materials and colorant‐free food decoration, to short‐term sensors in, for example, biodegradable “smart labels” for food packaging. A self‐supporting and structurally colored hydrogel is produced by combining hydroxypropyl cellulose (HPC) and gelatin in a scalable formulation process. By retaining the lyotropic, liquid crystalline behavior of the HPC into the gelled state, a spectrum of dynamic colors is produced. Rheological studies confirm a desirable non‐Newtonian shear‐thinning behavior and an increased stiffness, which result in a much quicker mechanochromic relaxation time.