LAUSR

Photonic materials with tunable structural colors in response to various stimuli have enabled diverse sensing and displaying applications. However, the changeable colors caused by mechanical deformations may severely confuse the optical readouts for the upcoming wearable photonics. Herein, an extremely stretchable supramolecular organogel is demonstrated with deformation‐insensitive structural colors through an unconventional cascade‐microphase‐separation process among the silica nanoparticles (SiO2 NPs), silicone oils, and hydrogen‐bonded polymer gel. The resultant sparse and abundant microscale SiO2 NP aggregates with proper sizes, shapes, and random distributions in the gel matrix serve as rigid structural color domains and secure invariant colors to the whole soft sample under extreme mechanical deformations. Moreover, the dynamic hydrogen bonding of the organogel matrix offers the nanocomposites shear‐thinning and easy‐molding property, making them ideal for color paints in versatile coating applications. The deformable organogel nanocomposites have great potentials in various fields requiring stable colors and open up a new avenue for the development of wearable photonic devices.