Abstract Profound understanding of relationships between molecular networks with properties can make it more convenient for people to prepare and employ shape memory polymers (SMPs). In this paper, a series of epoxy SMPs were developed based on epoxy (E‐51), trimethylolpropane tris(3‐mercaptopropionate) and pentaerythritoltetrakis (3‐mercaptopropionate), and 2‐methylimidazole, through “epoxy‐thiol” click reaction. The effect of networks on key properties (heat resistance and mechanical properties shape recovery performance) was systematically investigated. Experiment results indicated that there were positive correlations between network regularity with both thermal–mechanical properties and heat resistance. In addition, regularity of network structure had an effect to restrict shape recovery speed.
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