Chitosan　hydrogel　microspheres　derived　from　the　LiOH/KOH/urea　aqueous　system　demonstrate　great　characteristics　of　high　mechanical　strength,　relative　chemical　inertness,　renewability　and　3-D　fibrous　network,　making　them　promising　functional　supports.　This　work　aims　to　investigate　the　tunable　Co2+　adsorption　behaviors　on　these　robust　chitosan　microspheres　in　detail,　providing　the　theoretical　basis　for　optimizing　the　preparation　procedure　of　chitosan　microspheres　supported　Co3O4　catalysts　in　the　future.　The　experimental　results　revealed　that　the　fabricated　original　chitosan　microspheres　with　more　extended　chain　conformation　could　display　enhanced　adsorption　capacity　for　Co2+　at　determined　concentration　both　in　water　and　alcohol　solutions,　which　is　about　2-7　times　higher　than　that　of　the　conventional　chitosan　hydrogel　microspheres　prepared　from　the　acetic　acid　solution.　The　kinetic　experiments　indicated　that　the　adsorption　process　in　water　solution　agreed　with　the　pseudo-second-order　kinetic　equation　mostly,　while　the　chemical　and　physical　adsorptions　commonly　contribute　to　the　higher　Co2+　adsorption　on　chitosan　microspheres　in　alcohol　solution.　Moreover,　in　both　cases,　the　film　diffusion　or　chemical　reaction　is　the　rate　limiting　process　in　the　initial　adsorption　stage,　and　the　adsorption　of　Co2+　on　chitosan　microspheres　can　well　fit　to　the　Langmuir　isotherm.　Thermodynamic　analysis　demonstrated　that　such　adsorption　behaviors　were　dominated　by　an　endothermic　(ΔH°　＞　0)　and　spontaneous　(ΔG°　©　The　Royal　Society　of　Chemistry.