The　synthesis　of　crystalline　homochiral　MOF　materials　is　very　important　for　their　potential　application　in　enantioselective　processes　and　asymmetric　catalysis.　In　this　paper,　four　novel　zinc　based　chiral　boron　imidazolate　frameworks　(BIFs),　Zn-2[BH(2-eim)(3)](BA)(2)(OH)　(BIF-132-BA,　2-eim　=　2-ethylimidazolate,　BA　=　benzoate),　Zn　[HBH(2-ipim)(3)](OHBA)(Ac)　(BIF-133-OHBA,　2-ipim　=　2-isopropylimidazolate,　OHBA　=　o-hydroxybenzoate,　Ac　=　acetate),　Zn[HBH(2-ipim)(3)](PHBA)(Ac)　(BIF-133-PHBA,　PHBA　=　p-hydroxybenzoate),　and　Zn[HBH(2ipim)(3)](DHBA)(Ac)　(BIF-133-DHBA,　DHBA　=　2,4-dihydroxybenzoate)　were　prepared　via　solvothermal　synthesis.　Single-crystal　X-ray　diffraction　demonstrated　that　the　existence　of　hydrogen　bonds　between　adjacent　chains　results　in　two　different　structure　features　of　BIF-131:　a　chiral　ladder-like　1D　chain　(BIF-133-OHBA)　and　two　supramolecular　2D　layers　(BIF-133-PHBA　and　BIF-133-DHBA).　Then,　the　optical　activities　of　as-synthesied　crystals　were　preliminarily　studied　by　circular　dichroism　(CD)　spectroscopy.　In　addition,　because　they　crystallized　in　noncentrosymmetric　space　groups,　the　powder　second-harmonic　generation　(SHG)　measurements　were　carried　out　and　the　SHG　response　of　BIF-133-PHBA　was　almost　comparable　to　potassium　dihydrogen　phosphate　(KDP).