The　construction　of　hydrogen-bonded　organic　frameworks　(HOFs)　by　strong　intermolecular　hydrogen　bonding　interactions　has　received　much　attention　in　recent　years.　Different　from　common　reported　organic　molecules　based　HOFs,　we　demonstrate　here　the　Ni4L4　cubane　(L　​=　​S-1,2-bis(benzimidazole-2-yl))　containing　carboxylate　ligands　is　a　powerful　subunit　for　the　construction　of　HOFs.　In　this　subunit,　four　Ni2+　ions　are　coordinated　by　four　LH　ligands　to　form　typical　cubane　structure,　two　carboxylic　ligands　occupy　the　remaining　four　coordination　sites　in　bridging　mode.　Based　on　this　structure,　a　series　of　carboxylic　ligands　containing　potential　H-bond　sites　are　employed　to　control　the　self-assembly　of　Ni4L4　cubane　to　generate　different　HOFs　with　improved　stability　and　tunable　magnetic　properties.　©　2022　Elsevier　Inc.