The　development　of　multiple　metal-organic　framework　(MOF)　thin　films　with　high　lattice　mismatch　is　still　a　challenging　task.　Herein　we　report　a　series　of　single　and　multiple　(bi-varietal　and　tri-varietal)　pillar-layered　MOF　thin　films　(surface-coordinated　MOF　thin　films,　SURMOFs)　[Cu2L2dabco]n　(L　=　bdc,　bpc　and　tpdc)　with　preferred　[001]-orientation　on　the　substrate　surfaces　using　a　liquid-phase　epitaxial　(LPE)　layer　by　layer　pump　method.　The　single　SURMOFs　with　the　same　c-lattice　parameters　but　different　a-　and　b-lattice　parameters　result　in　the　successful　growth　of　oriented　multiple　SURMOFs　with　high　lattice　mismatch　(up　to　77.8%).　The　vapor　adsorption　results　show　that　the　representative　bi-varietal　SURMOF　with　large　lattice　mismatch　has　different　adsorption　behavior　from　single　SURMOFs,　providing　a　new　strategy　to　achieve　tuning　of　the　adsorption　kinetics　performance　in　sensing　applications.　©　2023　The　Royal　Society　of　Chemistry