N-nitrosodiethylamine　(NDEA)　is　a　disinfection　by-product　(DBP)　and　is　classified　as　a　probable　carcinogen　by　the　International　Agency　for　Research　on　Cancer.　Its　concentration　is　lower　but　its　toxicity　is　higher　than　other　DBPs.　Designing　a　new　adsorbent　with　a　high　adsorption　effect　on　low　concentrations　of　NDEA　instead　of　traditional　materials　will　be　useful.　To　the　best　of　our　knowledge,　this　is　the　first　study　to　investigate　metal-organic　frameworks　(MOFs)　for　the　adsorption　of　NDEA.　Two　novel　Al-based　MOFs　were　synthesized　by　modifying　MIL-96　with　amino　and　thiol　groups.　Their　adsorption　performances　at　low　concentrations　of　NDEA　in　water　were　compared　using　adsorption　kinetics　and　isotherm　models.　It　was　observed　that　MIL-96　modified　with　thiol　groups　(MIL-96-M)　followed　the　Langmuir　and　pseudo-second-order　models　and　exhibited　the　best　adsorption　performance.　Owing　to　the　well-matched　pore　size　and　hydrophobicity,　the　Langmuir　adsorption　capacity　of　MIL-96-M　for　NDEA　was　achieved　at　1004.71　μg/g.　The　parameters　of　the　adsorption　performance　were　investigated　using　the　Box-Behnken　response　surface　methodology,　and　on　the　basis　of　which,　the　performance　under　different　conditions　was　predicted.　The　experimental　data　suggested　that　the　increase　in　temperature　and　time　was　beneficial　for　the　adsorption　performance,　whereas　an　increase　in　dosage　was　not　beneficial.　It　was　identified　that　the　adsorption　mechanism　between　MIL-96-M　and　NDEA　involves　van　der　Waals　forces,　electrostatic　interactions,　and　nucleophilic　reactions　by　characterization　and　density　functional　theory　(DFT).　©　2022