Herein, we reported a sustainable and simple method involving electrochemical-catalyzed decarboxylative annulation and hydroaminomethylation of cyclic aldimines with N-arylglycines by switching the reaction solvents. When the reaction was carried out in MeCN/H2O or H2O, the resulting products included imidazolidine-fused sulfamidates and C4-aminomethylated cyclic aldimines, obtained in moderate to good yields, respectively. Mechanistically, a radical pathway was proposed to be involved in this approach.