Aseriesofamine-basedadsorbentsweresynthesizedusingsiliceousMCM-41inpiduallyimpregnatedwithfourdifferentamines(ethylenediamine(EDA),diethylenetriamine(DETA),tetraethylenepentamine(TEPA)andpentaethylenehexamine(PEHA))tostudytheeffectofaminechainlengthandloadingweightontheirCO2adsorptionperformancesindetail.TheadsorbentswerecharacterizedbyFT-IR,elementalanalysis,andthermo-gravimetricanalysistoconfirmtheirstructureproperties.Thermo-gravimetricanalysiswasalsousedtoevaluatetheCO2adsorptionperformanceofadsorbents.Longerchainamine-basedmaterialscanachievehigheramineloadingsandshowbetterthermalstability.TheCO2adsorptioncapacitiesatdifferenttemperaturesindicatethattheCO2adsorptionisthermodynamicallycontrolledoverEDAMCM41andDETA-MCM41,whiletheadsorptionoverTEPA-MCM41andPEHA-MCM41isunderkineticcontrolatlowtemperature.ThechainlengthofaminesaffectstheCO2adsorptionperformanceandtheadsorptionmechanismsignificantly.TheresultsalsoindicatethatCO2adsorptioncapacitycanbeenhanceddespiteofhighoperationtemperatures,ifappropriateamines(TEPAandPEHA)areapplied.However,adsorbentswithshortchainamineexhibithigheradsorptionanddesorptionratesduetothecollaborativeeffectofrapidreactionmechanismsofprimaryaminesandlessdiffusionresistanceofshorterchainlengthamines.