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An amino acid ionic liquid tetramethylammonium glycinate ([N1111]­[Gly]) and an organic supramolecular gelator N-lauroyl-l-glutamic acid di-n-butylamide (GP-1) were used as structure-directing agents for the fabrication of mesoporous alumina with diverse morphologies via a solvothermal synthetic method. The irregular sheets and hierarchical clusters were respectively prepared with only [N1111]­[Gly] or GP-1/EW as the template, whereas a distinct cactus rod-like morphology with interlaced lateral plates was constructed with [N1111]­[Gly] and GP-1 as the cotemplate. The cotemplate synergistic effects of [N1111]­[Gly] and GP-1 on the morphology tailoring of alumina have been investigated in depth. A self-assembly mechanism based on the bilayer arrangement model was proposed to be responsible for the formation of final cactus rod-like alumina. The intermolecular H-bonds between the GP-1 molecule and [N1111]­[Gly]-AlOOH hybrids was found to be the main driving force for the axial growth of initial nanocrystals, and the growth of the nanocrystals in lateral orientation was inhibited due to the stereohindrance effect of [N1111]­[Gly].