A new family of squarylium monoalkylamides and dialkylamides was synthesised and its organogelation ability was evaluated. We found that both squarylium monoalkylamides and dialkylamides formed organogels in DMF. We also found that ion-selective organogel formation was observed in DMF solutions containing metal ions, and gel electrolytes consisting of squarylium alkylamides, DMF and LiClO4 showed good ionic conductivities comparable to that of the corresponding liquid electrolytes.