Abstract: Six low-molecular-mass organic gelators were synthesized by the condensation reaction of sorbitol and derived benzenaldehyde with p-TsOH as catalyst.They are 1,3:2,4-dibenzylidene-D-sorbitol (DBS),1,3:2,4-di(4-methylbenzylidene)-D-sorbitol (MDBS),1,3:2,4-di(3,4-dimethylbenzylidene)-D-sorbitol (DMDBS),1,3:2,4-di(2,4,6-trimethylbenzylidene)-D-sorbitol(2,4,6-TMDBS),1,3:2,4-di(2,4,5-trimethylbenzylidene)-D-sorbitol (2,4,5-TMDBS) and 1,3:2,4-di(5,6,7,8-tetrahydronathalenyl-2-methylene)-D-sorbitol(DTNHS),and the yield is 30.9%~91.2%.Physical or chemical method was used to remove the water formed during the reaction.Structures of the targets were determined by ¹H NMR.Thermoreversible organogels were prepared with various organic solvent.The gel-sol phase transition temperature of gels was characterized by DSC.The structure of the gels were characterized by TEM and XRD.The results show that the 3D networks were formed in the gels.The diameter of the fiber affects the transparency of the gels.The gelator in gels were non-crystal in whole,but microcrystallite zones exist in the 3D networks.