The　application　of　cement-based　materials　in　engineering　requires　the　understanding　of　their　characteristics　and　subsequent　deformation　and　fracture　process　of　C-S-H　gel　in　service.　In　this　work,　three　types　of　amine　molecules　including　tetraethylenepentamine　(TEPA),　polyacrylamide　(PAM),　and　triethanolamine　(TEA)　were　intercalated　into　C-S-H　gel　in　an　unsaturated　status　successfully.　Systematical　analysis　was　performed　on　the　structures　and　properties　for　both　C-S-H　gel　and　corresponding　amine　molecules/C-S-H　gel.　It　was　found　that　the　unsaturated　intercalation　of　amine　molecules　into　C-S-H　gel　plays　a　key　role　in　the　geometry　and　therein　density　of　nanocomposites.　Subsequently,　radial　distribution　function　(RDF),　time-correlated　function　(TCF),　and　mean　square　displacement　(MSD)　were　applied　to　characterize　the　structure　and　dynamic　information　of　the　as-generated　nanocomposites,　demonstrating　the　occurrence　of　interaction　between　amine　molecules　with　Ca-Si　layer　and　acceleration　of　water　diffusion　by　unsaturated　intercalation　of　amine　molecules　into　the　interlayer　region　in　C-S-H　gel.　Finally,　the　deformation　and　fracture　process　of　C-S-H　gel　and　amine　molecules/C-S-H　gel　under　uniaxial　tensile　loads　were　given　by　molecular　dynamics　simulation.　It　was　indicated　that　the　tangent　modulus　of　nanocomposites　demonstrates　a　strain-softening　nature,　indicating　a　visco-elastic　behavior.　The　breakage　of　Ca-O　bonds　and　hydrogen　bonds　dominates　the　fracture　of　C-S-H　gel.　Weak　interaction　for　TEPA/C-S-H　gel　or　TEA/C-S-H　gel　leads　to　a　decreased　tensile　strength.　Local　stress　concentration　in　other　interlayer　region　governs　the　deformation　and　fracture　process　in　spite　of　the　formation　of　strong　interaction　between　double　bonded　polar　oxygen　atoms　in　PAM　molecules　and　Ca　atoms　in　C-S-H　gel.