Transient polymer networks, formed by polymer chains linked through reversible bonds, exhibit time-dependent viscoelasticity, that bridges solid-like elasticity and liquid-like flow. These materials have attracted increasing attention due to their potential for self-healing, toughness, and recyclability. Classical models, such as the Green–Tobolsky and Tanaka–Edwards theories, primarily describe stress relaxation by bond dissociation kinetics, assuming homogeneous equilibrium structures and small deformations. However, real-world applications often involve large, dynamic strains, where nonlinear viscoelasticity, finite extensibility, and spatial flow heterogeneity dominate. Conventional systems frequently suffer from structural and dynamic heterogeneities, complicating efforts to connect molecular dynamics with bulk mechanical behavior. To address these challenges, recent studies have developed a model transient network—Tetra-PEG slime—constructed from tetrafunctional polyethylene glycol (PEG) precursors connected via dynamic covalent bonds between phenylboronic acid and diol groups. This system allows for precise control over network connectivity, bond lifetime, and strand architecture, while minimizing unwanted heterogeneities. Leveraging this model, researchers have applied a multimodal approach, combining surface plasmon resonance (SPR), macroscopic rheology, two-dimensional rheo-optics, and particle-tracking microrheology to investigate relaxation behavior across linear and nonlinear regimes. These efforts have uncovered clear correlations between molecular kinetics and viscoelastic relaxation, time–strain separability under large deformations, damping mechanisms tied to strand pullout, and emergent spatial heterogeneity near the percolation threshold. This review summarizes these findings and explores their implications for the rational design of transient networks with programmable mechanical properties, while offering perspectives on future integrations with theory and simulation.
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