Oriented　metal-organic　framework　(MOF)　films　are　attracting　great　attention　due　to　their　fascinating　physicochemical　properties　and　unique　functionalities.　Here,　we　report　an　[110]-oriented　biomolecular　γ-cyclodextrin　(γCD)　MOF　film　with　arrayed　CD　channels　running　perpendicular　to　the　substrate　surface.　This　sophisticated　architecturewas　realized　by　combining　liquid　phase　epitaxial　layer-by-layer　(lbl)methods　with　a　γCD-based　thiol　self-assembled　monolayer　(SAM)　functionalized　surface.　This　first　demonstration　of　the　lbl　method　for　MOF　growth　from　aqueous　conditions　yielded　oriented,　highly　homogeneous,　and　chiral　γCD-SURMOFs　(surfacecoordinated　MOFs)　with　tunable　thickness.　Using　a　quartz　crystal　microbalance　(QCM)　to　monitor　adsorption　of　biomolecules,　we　demonstrated　that　γCD-SURMOF　provides　highly-efficient　recognition　of　tripeptide　enantiomers　(Tyr-(L-Ala)-Phe　vs　Tyr-　(D-Ala)-Phe),　clearly　outperforming　γCD(SH)8SAMs　as　well　as　polycrystalline,　mixed-orientations　γCDMOF　film.　The　presence　of　well-aligned　γCD-channels　enables　highly　efficient　transport　channels　with　large　adsorption　capacity　and　fast　loading,　along　with　high　enantioselectivity.　In　addition,　the　fast　and　highly　specific　loading　rates　allow　for　the　realization　of　highly　specific　sensors　for　biomolecules　with　short　response　times.　©　2022　The　authors.