Acentric　structure　is　the　indispensable　condition　for　a　compund　to　exhibit　nonlinear　optical　(NLO)　response.　However,　it＇s　difficult　for　inorganic　sulfates　to　crystallize　in　acentric　structures.　In　this　communication,　a　new　acentric　sulfate,　Cs2Zn2(SO4)(3),　has　been　synthesized　by　spontaneous　crystallization　method.　The　crystal　structure　of　Cs2Zn2(SO4)(3)　is　layered　and　is　composed　of　Zn-2(SO4)(3)　layers　and　Cs+　cations,　which　is　different　from　A(2)B(2)(SO4)(3)　(A　=　K,　Rb,　B　=　Mg,　Ca,　Cd,　Zn)　type　that　owns　three-dimensional　framework.　Powder　NLO　response　suggest　that　Cs2Zn2(SO4)(3)　exhibits　a　moderate　second-order　NLO　response　of　about　0.15　x　KH2PO4.　Theoretical　calculations　were　performed　and　elucidated　that　the　origination　of　NLO　response　is　from　SO4　groups　and　ZnOn　(n　=　4,　5)　polyhedra.　This　work　will　enrich　the　diversity　of　sulfate　structure　and　provide　new　desgin　strategy　on　the　synthesis　of　novel　NLO　sulfates.