Although tremendous research investigations on organogelators and hydrogelators have been conducted, the reports about the ambidextrous gelators capable of gelating both organic solvents, especially, apolar solvents and water are very limited. In order to create efficient ambidextrous gelators it should be necessary to take a bottom‐up approach. Thus, according to molecular design the amphiphilic compounds consisting of glutamate‐based structure having two long alkyl chains and the ethanolamine moiety have been prepared. The compounds having C6 and C7 alkyl chains have been found out to work as an excellent ambidextrous capability because they can only gelate water and apolar solvents. Although the compounds having C9 and C10 alkyl chain showed no gelation in water, by introduction of an ammonium cation into these compounds ambidextrous properties were gained. Ambidextrous ability can be imparted to the compound having no ambidextrous properties by mixing with a small amount of an authentic ambidextrous gelator.