Sulfur-containing polyurea compositions comprising a polyisocyanate and a polyamine are disclosed. The polyisocyanate comprises the reaction product of reactants comprising a diisocyanate having isocyanate groups with different reactivities toward thiol groups, and a thiol-terminated sulfur-containing polymer such as a thiol-terminated polythioether polymer and/or a thiol-terminated polyformal polymer. The polyamine can be an aromatic polyamine and/or an aromatic amine-terminated polythioether adduct. The sulfur-containing polyurea compositions are useful as aerospace sealants.