Pyrrole was found to be polymerized to conducting polypyrrole by solution-surface (SS) electropolymerization in which the polymerization occurs along the solution-gas interface or along the interface between aqueous and nonaqueous solvents. The SS polymerization of pyrrole was observed to occur with various electrolytes in aqueous solutions in contact with a gas phase or an organic phase. Conditions favorable for SS polymerization were examined. The SS polymerization seemed to require, among other things, a large surface (interfacial) tension of the solvent which is a prerequisite for surface excess of the monomer at the interface.