Biological soft materials found in nature have complex structures that allow them to function in demanding scenarios. For example, the balanced combination of hydrophilic and hydrophobic segments in elastic biopolymers, such as in resilin, led to remarkable mechanical properties, including high stretchability and resilience, which are exploited in nature by many species for mechanical energy storage to facilitate their movement. Developing a synthetic material with resilin-like properties requires high stretchability to store elastic energy, low hysteresis for high energy conversion, and high retraction velocity when released from a stretched state for power amplification. Here, we present the synthesis and characterization of hydrogels capable of mimicking some of these properties. These gels are synthesized through a single-step free-radical polymerization of hydrophilic acrylic acid, alkyl-acrylamide, for example, methylacrylamide (MAM), and hydrophobic poly(propylene glycol) diacrylate [PPGDA]. By changing the chemical compositions, the modulus of these gels can be tuned from 10 to 100 kPa, and the stretchability from 2 to 11 times their original length. Also, these gels display low dissipation, retract rapidly to their original length when released from a stretched state, and are also stable in saline environments. All these properties make these gels suitable for many biomimetic applications, including in soft robots. Another important characteristic of biological tissues is strain-stiffening behavior that protects them from injury. Similar strain-stiffening behavior can be obtained for synthetic gels of ABA triblock copolymers in a B-block selective solvent, making them attractive candidates in many applications, from personal products to ballistic applications. Capturing the structure evolution as a function of applied strain provides insight into the microstructure-dependent mechanical properties of these gels. Here, we present the strain-dependent transient microstructure of ABA triblock copolymer gels captured using combined rheology and scattering (RheoSAXS) experiments. The large amplitude oscillatory strain was applied to these gels, and the microstructural evolution in a given strain cycle was captured. The polymer concentration, solvent quality, and midblock length play a role in these gels' rheological behavior and microstructure evolution. Our study captures unique structure-properties relationships for polymer gels important for their applications in many areas of interest.