Reverse　osmosis　(RO)　has　been　recognized　as　a　reliable　technique　for　wastewater　reclamation.　To　enhance　its　rejection　of　trace　organic　contaminants　(TrOCs),　a　novel　strategy　was　proposed　to　improve　reverse　osmosis　(RO)　membranes　by　fabricating　thin-film　nanocomposite　membrane　(TFNi)　with　a　TA-Fe3+/CNTs　interlayer.　The　TFNi-30　membrane　was　obtained　by　optimizing　the　loading　capacity.　This　optimized　membrane　gave　rise　to　an　enhanced　water　permeance　of　3.2　±　0.2　L　m-2　h-1　bar-1,　which　was　two　times　higher　than　that　of　the　control　membrane　(1.1　±　0.2　L　m-2　h-1　bar-1),　while　achieving　a　considerably　higher　rejection　of　inorganic　salts　and　trace　organic　contaminants　(TrOCs)　thanks　to　the　formation　of　a　denser　polyamide　rejection　layer.　In　addition,　the　specific　roles　of　the　interlayer　structure　in　determining　the　separation　performance　of　RO　membranes　were　investigated　by　tailoring　the　support-free　RO　membranes　and　comparing　them　with　the　conventional　membranes.　This　study　would　provide　a　peer　reference　for　designing　high　performance　RO　membranes　for　wastewater　reclamation　via　the　TFNi　strategy.　©　2023　Elsevier　B.V.