Graphene　oxide　(GO)　has　been　considered　as　a　promising　material　to　develop　advanced　nanofiltration　membranes　to　resolve　the　current　worldwide　water　scarcity　issue,　benefiting　from　its　extraordinary　physicochemical　properties.　However,　loose-GO-nanosheet-stacking　rendered　membrane　compaction　during　operation　significantly　harms　the　mass　transfer　of　GO　membranes.　Here,　we　proposed　an　ice-crystal　templating　approach　to　simultaneously　tailor　the　two　mass　transfer　channels　of　GO　membranes,　i.e.,　nanochannels　originated　from　the　interlayer　spacing　and　microporous　defects　arising　from　poorly　stacking　of　nanosheets.　The　tunability　of　the　ice-crystal　templating　strategy　was　verified　by　low-field　nuclear　magnetic　resonance　(LF-NMR)　coupled　with　X-ray　diffraction　patterns　technique.　The　result　demonstrated　that　the　interlayer　spacing　can　be　precisely　tuned　from　7.5　to　9.3　A　while　the　volume　of　microporous　defects　can　be　adjusted　from　2.9%　to　24.6%.　Thus,　the　optimized　GO　membrane　(M2)　was　utilized　for　desalination　of　dye/NaCl　mixtures　and　accomplished　a　high　separation　performance,　for　example,　high　water　permeability　of　similar　to　22.6　LMH/bar　(10-fold　enhancement　compared　with　traditional　GO　membranes),　100%　rejection　to　EB　dyes,　19%　rejection　to　NaCl,　and　long-term　running　stability　(180　h).　Therefore,　the　innovative　ice-crystal　templating　fabrication　techniques　opens　the　door　for　the　design　of　high-efficiency　2D　material-based　membranes.　(C)　2021　Elsevier　Ltd.　All　rights　reserved.