A　novel　adsorbent　of　AgBr-AgBr/CTAB　nano　materials,　which　was　synthesized　via　Tollen＇s　reagent　with　the　aid　of　hexadecyltrimethy　ammonium　bromide　(CTAB),　showed　an　excellent　high　affinity　to　anions　and　was　used　for　removal　of　organic　dyes　in　aqueous　solutions.　The　synthesized　AgBr-AgBr/CTAB　was　thoroughly　characterized　by　XRD,　SEM,　TEM,　XPS,　FTIR,　TGA,　DLS　as　well　as　zeta　potential　measurements.　The　adsorption　property　and　capacity　of　AgBr-AgBr/CTAB　for　organic　dyes　were　evaluated　using　methylene　blue　(MB),　rhodamine　B　(RhB),　acid　red　18　(AR-18),　orange　G　(OG),　indigo　carmine　(IC),　and　methyl　orange　(MO)　as　models.　The　adsorption　capacity　of　AgBr-AgBr/CTAB　complex　toward　four　anionic　dyes　OG,　AR-18,　IC,　and　MO　solutions　was　87.43　+/-　2.03　mg　g(-1),　205.89　+/-　2.12　mg　g(-1),　140.42　+/-　2.13　mg　g(-1),　and　104.6　+/-　1.59　mg　g(-1),　respectively.　On　the　other　hand,　this　adsorbent　exhibited　little　adsorption　ability　toward　two　cationic　dyes,　MB　(2.99　+/-　0.40　mg　g(-1))　and　RhB　(2.96　+/-　0.60　mg　g(-1)).　Interestingly,　AgBr-AgBr/CTAB　could　be　applied　to　efficiently　adsorb　anionic　dyes　from　binary　cationic-anionic　dye　systems　with　a　high　separation　factor,　and　such　adsorbent　could　be　reused　at　least　5　times　with　adsorption　capacities　above　95%.　The　removal　of　anionic　dyes　followed　pseudo-first-order　kinetics　and　Langmuir　isotherm　model,　indicating　that　anionic　dyes　were　monolayerly　adsorbed　on　our　as-prepared　materials.　To　further　elucidate　the　adsorption　mechanism,　the　theoretical　calculation　based　on　first-principles　was　also　provided.　The　results　suggested　R-SO3-　groups　were　the　active　sites　and　electrostatic　attraction　was　the　dominating　contribution　for　the　adsorption　of　anionic　dyes.