The physical aging of poly(urethanes) containing metal ions introduced by different methods (doping with a metal-containing active filler or chemical binding to PU chains) was studied by EPR, dynamic relaxation spectroscopy, and surface tension measurements. The method of introducing metal ions into PU samples affects both their characteristics immediately upon the synthesis and the long-term variation of their properties, including manifestations of the so-called surface aging. In the PU samples studied, the process of physical aging is related to a change in the content of various structures formed as a result of the intermolecular interactions controlled by metal ions.