Heavy　metal　ions　pollution　has　caused　worldwide　attention　due　to　its　toxicity　to　people＇s　health.　Existing　as　chromate　anions,　Cr(VI)　is　difficult　to　remove　from　polluted　water.　Owing　to　their　low　cost,　stability,　environmentally　benign　nature,　and　excellent　properties,　silicate　materials　are　widely　used　in　catalysis　and　adsorption.　In　this　work,　magnesium　silicates　with　sepiolite　and　talc　phase　were　synthesized　through　facile　hydrothermal　route　using　diatomite　as　substrate　and　silicon　source.　The　Cr　removal　capacity　of　wire-like　Mg4Si6O15(OH)2diatomite　exhibited　a　Cr　adsorption　capacity　of　1292　mg/g,　which　was　much　higher　than　the　other　reported　inorganic　adsorbents.　The　adsorption　followed　Freundlich　and　Temkin　models　well,　indicating　that　Cr　species　adsorbed　onto　adsorbent　was　a　favorable,　exothermic　multilayer　chemisorption　process.　The　first-principles　density　functional　theory　(DFT)　calculation　results　revealed　the　interaction　between　adsorptive　sites　of　adsorbents　and　Cr　species,　also　demonstrated　ion-exchange　behavior　between　interlayer　Mg　ion　and　Cr(III).　We　believe　these　low-cost　synthesized　adsorbents　have　great　potentials　for　practical　applications　in　the　treatment　of　heavy　metal　ions　polluted　wastewater.