The　layered　double　hydroxide　(LDH)　nanosheets　are　ideal　for　photocatalytic　CO2　reduction.　How　to　suppress　the　spontaneous　agglomeration　of　LDH　remains　a　challenge.　Herein,　this　work　reports　that　the　insulated　calcium　silicate　hydrate　(CSH)　nanosheets　effectively　suppress　the　agglomeration　of　NiAl-LDH　nanosheets　by　an　electrostatic　self-assembly.　The　charge　transfer　of　NiAl-LDH/CSH　is　effectively　promoted,　as　verified　by　photoelectrochemical　characterizations.　As　a　result,　the　CO　and　H2　generation　rates　from　photocatalytic　CO2　reduction　are　as　high　as　3432　and　1411　μmol　g−1h−1,　which　are　∼2.4　times　higher　than　that　of　the　pure　NiAl-LDH.　©　2023　Elsevier　B.V.