Noncovalent　interactions　are　ubiquitous,　endowing　high　feasibility　on　assembly　and　disassembly　of　gel　network　structure.　Loading　anticancer　drugs　in　low　molecular　weight　gelator　(LMWG)-based　gel　through　a　noncovalently　co-assembly　process　shows　advantages　of　high　efficacy,　thixotropy,　and　controllable　release.　Drug-loaded　fluorenylmethyloxycarbonyl-phenylalanine　(Fmoc-F)/DMSO/H2O-doxorubicin　(DOX)　gels　were　fabricated　by　an　effective　solvent-triggering　method　dominated　by　solvated　Fmoc-F　with　DMSO.　Density　Functional　Theory　(DFT)　calculation　results　show　that　the　noncovalent　interactions　between　Fmoc-F　and　DOX　drive　the　co-assembly　of　the　gel.　DOX　can　assemble　with　Fmoc-F　and　realize　its　co-assembly　loading　through　the　H-bonding　and　π-π　stacking,　similar　to　the　way　that　gel　networks　form.　Depending　on　a　network　dis-assembly　process,　sustained　release　of　DOX　was　achieved　along　with　carrier　decomposition　through　a　repetitive　diffusion-surface　erosion　process.　DOX　loading　and　release　prove　the　non-covalent　interactions　and　the　mechanism　for　controlling　the　assembly　process.　By　such　tailoring　co-assembled　loading,　the　administration　of　DOX　is　hoped　to　be　optimized　to　improve　the　clinical　application.　©　2022　Elsevier　Inc.