A novel, effective asymmetric 1-glycyl-3-methyl imidazolium chloride–iron(III) [[Gmim]Cl–Fe(III)] complex was synthesized and studied as organocatalyst in asymmetric aldol addition under solvent free condition at 25 °C. The hydrophobic group of amino acid favors reagent diffusion toward the chloroglycine moiety increasing the catalytic activity of supported iron complex. This method contains simplified product isolation and catalyst recycling, affording substituted aromatic aldehydes imparting high yield of aldol with excellent stereo-selectivity. This recyclable heterogeneous catalyst provides a simple strategy for the generation of a variety of new Csingle bondC bonds under environmentally benign condition.