The　amine　(NH2)-functionalized　UiO-66　was　successfully　anchored　on　disorderly　layered　clinoptilolite　(CP)　via　surfactant　(poly(ethylene　glycol)　(PEG)　and　poly(vinylpyrrolidone)　(PVP))-assisted　induction.　The　structural　features　and　physicochemical　parameters　of　the　resultant　UiO-66-on-CPs　were　characterized　by　powder　X-ray　diffraction　(XRD)　patterns,　scanning/transmission　electron　microscopy　(SEM/TEM)　images,　Fourier　transform　infrared　(FT-IR)　spectra,　N-2　sorption　isotherms,　and　small-angle　X-ray　scattering　(SAXS)　patterns.　The　results　demonstrated　that　the　growth　of　UiO-66-NH2　nanoparticles　facilitated　the　disorder　degree　of　the　crystal　plane　of　CP　along　the　a-axis,　while　the　addition　of　PEG　in　the　hydrothermal　synthesis　system　of　CP　was　conducive　to　the　formation　of　a　flower-like　microstructure　and　the　introduction　of　PVP　was　beneficial　to　the　nucleation　and　growth　of　UiO-66-NH2　nanoparticles　with　a　small　size　(40　nm)　on　the　surfaces　of　the　obtained　CP-PEG　lamellas.　Finally,　the　gas-selective　adsorption　and　separation　performances　of　CO2　and　CH4　were　evaluated　using　the　synthesized　disorderly　layered　UiO-66-on-CP　heterostructures　as　adsorbents,　indicating　that　the　NH2-functionalized　UiO-66-on-CP　exhibited　a　superior　selective　factor　(3.66)　of　CO2/CH4.　These　results　elucidated　that　the　proposed　approach　is　a　promising　strategy　for　constructing　MOF-on-zeolite　heterostructures,　which　may　open　an　avenue　to　expand　CP　application　and　improve　their　performance.