In　epoxy-amine　based　self-healing　cement-based　materials,　the　uncontrollable　stoichiometric　ratio　of　both　components　in　the　cracks　leads　to　the　cured　epoxy　resin　with　various　crosslink　densities.　Investigation　on　the　interaction　mechanism　between　cured　epoxy　resin　and　C-S-H　gel　promotes　to　optimize　the　final　self-healing　performances.　In　this　work,　the　interaction　between　load-induced　broken　panels　of　C-S-H　gel　and　cured　epoxy　resins　with　different　crosslink　densities　(e.g.,　0.23,　0.77,　and　0.97)　was　studied　through　molecular　dynamic　methods.　It　was　found　that　crosslink　density　plays　an　essential　role　in　the　geometrical　size　and　atom　distributions.　Phase　separation　occurs　at　the　low　crosslink　density　due　to　the　aggregation　of　amine　molecules.　The　generation　of　fresh　crosslink　points　limits　the　free　motion　of　epoxy　molecules　with　higher　crosslink　density.　Meanwhile,　the　cured　epoxy　resin　with　higher　crosslink　density　causes　a　high　porosity　in　the　interfacial　region　between　the　epoxy　resin　and　C-S-H　gel　substrates,　degrading　the　mechanical　performance　of　materials.