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In this study, we unravel the atomic structure of a covalent resin near boundaries such as surfaces and composite constituents. For this, a molecular simulation analysis of epoxy resin hardening under various boundary conditions was performed. On the atomic level of detail, molecular dynamics simulations were employed to study crosslinking reactions and self-organization of the polymer network within nm scale slab models. The resulting structures were then coarsened into a graph theoretical description for connectivity analysis of the nodes and combined with characterization of the node-to-node vector orientation. On this basis, we show that the local bonding of epoxy resins near interfaces tends to avoid under-coordinated linker sites. For both epoxy–vacuum surface models and epoxy–silica/epoxy cellulose interfaces, we find almost fully cured polymer networks. These feature a local increase in network linking lateral to the surface/interface, rather than the dangling of unreacted epoxy groups. Consequently, interface tension is low (as compared to the work of separating bulk epoxy), and the reactivity of the resin surface appears negligible.