Two　unusual　nanotube-based　boron　imidazolate　frameworks　(BIF-134　and　BIF-135)　were　synthesized　by　a　dual-ligand　synthetic　strategy　under　solvothermal　conditions.　In　the　structure　of　BIF-134　([Co(BH(2-mim)3)(BTC)1/3](HBH(2-mim)3)1/3(NMA);　2-mim　=　2-methylimidazole,　NMA　=　N-methylacetamide,　and　BTC　=　1,3,5-benzene　tricarboxylate),　one　part　of　boron　imidazolate　ligands　participate　in　the　structural　skeleton　coordination,　while　another　part　of　boron　imidazolate　ligands　act　as　guest　molecules　that　are　located　between　adjacent　nanotubes,　which　enhance　the　stability　of　the　framework　by　the　host-guest　interaction　and　the　pore　space　partition　effects.　It　was　found　to　be　highly　stable　in　air,　water,　organic　solvents,　and　a　wide　pH　range　(pH　0-12).　However,　in　the　structure　of　BIF-135　([Zn(BH(2-mim)3)(CHTC)1/3];　CHTC　=　1,3,5-cyclohexanetricarboxylate),　all　boron　imidazolate　ligands　participate　in　the　structural　skeleton　coordination;　there　is　no　boron　imidazolate　guest　molecule　in　the　pores.　The　topology　of　BIF-135　is　similar　to　that　of　BIF-134　by　replacing　BTC　with　CHTC　and　replacing　Co　with　Zn.　Furthermore,　the　obtained　BIFs　exhibited　third-order　nonlinear　optical　properties　and　potential　optical　limiting　applications　demonstrated　by　reverse　saturable　absorption.　©　2022　American　Chemical　Society.