The　constructed　strategy　of　the　disorderly　layered　UiO-66-on-clinoptilolite　heterostructures　was　proposed　through　assistance　of　polyethylene　glycol　(PEG)　and　polyvinylpyrrolidone　(PVP).　Their　physicochemical　properties　were　demonstrated　via　various　characterizations,　such　as　X-ray　powder　diffraction　(XRD)　patterns　and　scanning/transmission　electron　microscope　(SEM/TEM)　images.　Particularly,　the　small-angle　X-ray　scattering　(SAXS)　method　was　employed　to　elucidate　their　fractal　structure　evolutions,　manifesting　the　transformations　of　surface　fractal　with　irregularity　and　roughness.　The　results　showed　that　the　PEG　introduction　was　beneficial　to　the　formation　of　disorderly　layered　clinoptilolites　(CP).　The　particles　sizes　of　UiO-66-NH2　were　successfully　controlled　via　additive　PVP,　and　the　interactions　between　UiO-66-NH2　and　deposited　CP-PEG　were　enhanced.　The　preliminarily　adsorption　performances　of　the　obtained　UiO-66-on-CPs　exhibited　a　superior　selective　factor　(around　26)　of　CO2/CH4.　This　approach　may　open　a　new　avenue　to　improve　its　adsorption　selective　performance　for　CO2　and　CH4　due　to　its　dual　microporous　features　and　enlarged　lamellar　spacing.