Divergent Deborah number-dependent transition from homogeneity to heterogeneity.

Heterogeneous structures are ubiquitous in natural organisms. Native heterogeneous structures inspire many artificial structures that are playing important roles in modern society, while it is challenging to identify the relevant factors in forming these structures due to the complexity of living systems. Here, hybrid hydrogels consisting of flexible polymer networks with embedded stiff cellulose nanocrystals (CNCs) are considered an open system to simulate the generalized formation of heterogeneous core-sheath structures.