The　random　lamellae　of　the　synthetic　CP　were　synthesized　with　a　hydrothermal　approach　using　o-Phenylenediamine　(OPD)　as　a　modifier.　The　decreases　in　the　order　degree　of　the　CP　synthesized　in　the　presence　of　the　OPD　resulted　from　the　loss　of　long-range　order　in　a　certain　direction.　Subsequently,　the　ultrasonic　treatment　and　washing　were　conducive　to　further　facilitate　the　disordered　arrangements　of　its　lamellae.　The　possible　promotion　mechanism　regarding　the　nucleation　and　growth　behaviors　of　the　sol-gel　particles　was　proposed.　The　fractal　evolutions　of　the　aluminosilicate　species　with　crystallization　time　implied　that　the　aluminosilicate　species　became　gradually　smooth　to　rough　during　the　crystallization　procedures　since　the　amorphous　structures　transformed　into　flower-like　morphologies.　Their　gas　adsorption　and　separation　performances　indicated　that　the　adsorption　capacity　of　CO2　at　273　K　reached　up　to　2.14　mmol　&　BULL;g(-1)　at　1　bar,　and　the　selective　factor　(CO2/CH4)　up　to　3.4,　much　higher　than　that　of　the　CPs　synthesized　without　additive　OPD.　The　breakthrough　experiments　displayed　a　longer　breakthrough　time　and　enhancement　of　CO2　uptake,　showing　better　performance　for　CO2/CH4　separation.　The　cycling　test　further　highlighted　their　efficiency　for　CO2/CH4　separation.