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Novel mono- and dinuclear dimethyltin(IV) complexes were synthesized using tridentate Schiff base ligands, derived from 2-amino-2-hydroxymethyl-propane-1,3-diol and various aldehydes. These diorganotin(IV) compounds displayed good catalytic activity for solvent-free cycloaddition of CO2 to epoxides at ambient pressure. These catalysts efficiently completed the insertion of CO2 to various epoxides at low catalyst loadings (0.1–1.0 mol%) in 1–6 hours giving high values of TONs around 1000. The catalyst further usability for three continuous reaction runs in the reaction mixture gives the same activity revealing the remarkable stability of these compounds under the given reaction conditions. Therefore, organotin(IV) complexes are efficient catalysts for the synthesis of the industrially important cyclic carbonates from epoxides at ambient pressure under solvent-free conditions.