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• Two novel organogels were synthesized which alkyl chains of different lengths. • Non-covalent bond provide a good driving force for gel self-assembly. • The Zn2+ responsiveness experiment is completed and confirmed by UV spectrum. Two Salen type Schiff based on o-phenylenediamine were synthesized. The prepared organogelators demonstrated excellent gel properties in some selected solvents, such as n-pentanol, chloroform, and 1,2-dichloroethane. The results for thermal stability showed that under concentrations increasing of the gel molecules and then the gel-to-sol transition temperature value is increased. Through various techniques found that the hydrogen bonding between molecules, the van der Waals force, and the π-π stacking provide multiple driving forces for gel self-assembly. The morphology of the xerogel was investigated by Scanning Electron Microscope (SEM). The metal ions responsiveness experiment is completed by adding the metal ions solution dropwise to the gel surface and confirmed by the UV spectrum. [ABSTRACT FROM AUTHOR]