Tailoring smart hydrogels through manipulation of heterogeneous subdomains

The mechanical interactions among integrated cellular structures in soft tissues dictate the mechanical behaviors and morphogenetic deformations observed in living organisms. However, replicating these multifaceted attributes in synthetic soft materials remains a challenge. In this work, we develop a smart hydrogel system featuring engineered stiff cellular patterns that induce strain-driven heterogeneous subdomains within the hydrogel film. These subdomains arise from the distinct mechanical responses of the pattern and film domains under applied mechanical forces. Unlike previous studies that incorporate reinforced inclusions into soft matrices to tailor material properties, our method manipulates the localization, integration, and interaction of these subdomain building blocks within the soft film. This enables extensive tuning of both local and global behaviors. Notably, we introduce a subdomain-interface mechanism that allows for the concurrent customization and decoupling of mechanical properties and shape transformations within a single material system—an achievement rarely accomplished with current synthetic soft materials. Additionally, our use of in-situ imaging characterizations, including full-field strain mapping via digital imaging correlation and reciprocal-space patterns through fast Fourier transform analysis of real-space pattern domains, provides rapid real-time monitoring tools to uncover the underlying principles governing tailored multiscale heterogeneities and intricate behaviors.