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 as an open system to simulate the generalized formation of heterogeneous core-sheath structures, which are formed as the dynamic response to external environment. As the result of environmental adaption during modified air drying processes of hybrid hydrogels, the formation of heterogeneous core-sheath structure was found to be correlated to the relative evaporation speed. The formation of such heterogeneity in xerogel fibers was found to be correlated with Deborah number (De). During the transition of De from large to small values with accompanying morphologies, the turning point was around De = 1. The mechanism can be considered a relative humidity-dependent glass transition behavior. These unique heterogeneous structures play a key role in tuning water permeation and water sorption capacity. Insights into these aspects can prospectively contribute to a better understanding of the native heterogeneous structures for bionics design.