Gas　adsorbent　demonstrates　a　high　importance　in　the　reduction　of　CO2　emission　while　graphene　oxide　(GO)　is　a　promising　2D　material　for　CO2　adsorption　for　its　high　theoretical　surface　area　and　abundant　oxygen-containing　functional　groups　distributed　on　the　2D　nanosheet.　However,　the　current　gas　adsorption　capability　lags　largely　behind　the　ideal　value,　arising　from　the　aggregation　and　restacking　of　GO　nanosheets　hindering　the　exposure　of　adsorption　sites.　Here,　the　‘ionic-crosslinking　induced　dynamic　assembly　coupled　ice-templating’　(IDAI)　strategy　was　employed　to　fabricate　the　porous　3D　GO　framework　for　CO2　capture,　which　could　alleviate　the　aggregation　and　restacking　issue　of　GO　nanosheets　during　fabrication　by　the　ionic　crosslinking.　The　fabricated　3D　GO　microstructure　can　be　adjusted　by　controlling　the　dynamic　assembly　process　by　changing　the　GO　concentration.　After　optimization,　the　porous　3D　GO　adsorbent　offers　a　CO2　adsorption　capacity　of　2.24　mmol/g　at　ambient　pressure　and　temperature　with　good　running　stability,　attributed　to　the　strong　ionic　crosslinking.　More　importantly,　the　proposed　method　shows　the　generality　of　many　multivalent　cations,　which　constructs　a　versatile　platform　for　GO　microstructure　tailoring.　©　2023　Elsevier　B.V.