Five low molecular-mass organic gelators were synthesized by condensation of xylitol and different derived benzaldehydes using dodecyl benzenesulfonic acid as catalyst and removing water by azeotropic distillation with cyclohexane. They are: 1,3:2,4-O-bis(4-methylbenzylidene)–D-xylitol(1),1,3:2,4-O-bis(3-methylbenzylidene)–D-xylitol(2),1,3:2,4-O-bis(2-methylbenzylidene)–D-xylitol(3),1,3:2,4-O-bis(3,4-dimethylbenzylidene)-D-xylitol(4),1,3:2,4-O-dibenzylidene-D-xylitol(5). For the first time xylitol acetal were used as gelator. The performance of gelation were tested using 34 kinds of organic solvents. The substituents of the benzene ring may affect the ability of gellation, Some of them can enhance the interaction of the gelator molecular. The solvent molecular participate the formation of 3-D network. As for most xylitol acetal gelators, H-bond play the key role in the self-assembly.