Superhydrophilic　poly(ethyleneimine)/poly(sodium-4-styrenesulfonate)　(PEI/PSS)-calcium　silicate　hydrate　(CSH)　multilayered　membranes　(PEI/PSS)(2.0)(PEI/PSS-CSH)(n)　on　polyacrylonitrile　(PAN)　substrate　were　prepared　via　layer-by-layer　(LbL)　assembly　with　in　situ　precipitation　of　consecutive　Ca2+-integrated　multilayered　polyelectrolytes　and　sodium　silicate.　The　surface　structure　and　properties　of　these　multilayered　membranes　(PEI/PSS)(2.0)(PEI/PSS-CSH)(n)　were　characterized　by　zeta　potential,　infrared　resonance　spectra,　water　contact　angles,　scanning　electron　microscopy,　and　atomic　force　microscopy,　and　the　separation　performances　were　evaluated　by　rejection　of　dyes,　such　as　xylenol　orange　(XO)　and　rhodamine　B　(RB).　The　long　term　performance,　self-cleaning　and　antifouling　behaviors　were　investigated　by　retention　of　aqueous　solutions　of　both　dyes　and　bovine　serum　albumin　(BSA)　aqueous　solution.　The　results　indicated　that　the　in　situ　incorporation　of　controlled　CSH　contents　into　PEI/PSS　multilayers　greatly　improved　the　hydrophilicity　of　the　multilayered　membranes,　resulting　in　the　formation　of　a　superhydrophilic　(PEI/PSS-CSH)(2.0)　membrane　with　a　water　contact　angle　of　2.1　degrees　and　the　highest　permeate　fluxes　of　191.5　and　183.5　L　m(-2)　h(-1)　MPa-1　accompanied　by　the　rejection　of　94.0%　and　91.2%　for　XO　and　RB　aqueous　solutions,　respectively.　When　the　number　of　assembled　(PEI/PSS-CSH)(n)　multilayers　was　higher　than　2.0　bilayers,　the　rejection　increased　but　the　flux　markedly　decreased　to　XO　and　RB　dyes,　showing　a　characteristic　trade-off　phenomenon.　Moreover,　the　superhydrophilic　(PEI/PSS-CSH)(2.0)　membrane　possessed　a　higher　antifouling　and　self-cleaning　behavior　than　the　hydrophilic　polyelectrolytes　(PEI/PSS)(2.0).