With　the　assistance　of　cetyltrimethyl　ammonium　bromide　(CTAB),　the　delamination　of　disorderly　layered　cli-noptilolite　(CP)　was　performed.　The　introduction　of　CTAB　in　hydrothermal　system　was　beneficial　to　stratification　of　CP　lamellas　by　enlarging　interlayer　spacing,　and　thus　accelerating　the　formation　of　disordered　CP　nanosheets.　The　hydrophobic　alkyl　chain　restricts　the　crystal　growth　along　a-axis　and　the　few-layer　CP　lamellas　with　inte-grally　preserved　heulandite　structures　were　obtained　by　ultrasonic　treatment　and　HNO3　modification　at　room　temperature.　Meanwhile,　the　CTAB-assisted　crystallization　mechanism　was　further　elucidated,　in　which,　the　amorphous　spherical　nanoparticles　were　firstly　generated　and　then　transformed　into　the　fibrous　and　lamellar　species.　Finally,　the　flower-like　CP　morphologies　with　the　aggregated　nanosheets　appeared.　Meanwhile,　the　selective　adsorptions　and　separations　of　CO2　and　CH4　using　these　delaminated　CPs　as　the　absorbents　were　preliminarily　explored,　showing　a　strong　potential　in　the　mixed　gases　separation　applications.　This　approach　is　a　promising　strategy　for　constructing　delaminated　zeolites　with　low　n(SiO2/Al2O3),　which　may　open　a　new　avenue　for　the　delaminated　CP　nanosheet　applications　in　gas　adsorption　and　separation　fields.