A series of two-component polymer networks consisting of poly(tetrahydrofuran) [poly(THE)I and polystyrene segments (3) was produced through a macromolecular ion-coupling reaction between telechelic poly(THF) having pyrrolidinium salt groups (1) of various molecular weights, and a series of poly(styrene-co-tetrabutylammonium acrylate) (2) having carboxylate contents of up to ca. 20 mol%. The coupling reaction proceeded efficiently by simple coprecipitation of a THF solution of an equivalent mixture of 1 and 2 into cold water to combine the two prepolymers by Coulombic interaction. The subsequent heat treatment of the ionically linked pseudo-network product led to covalently linked, permanent network polymers consisting of the two different segment components. The equilibrium swelling degree of a series of network copolymers in toluene was found to be controllable either by the molecular weight of 1 or by the carboxylate content of 2.