A series of polyurethane/PMMA simultaneous interpenetrating networks (SINs) with various hard segment contents (X) in the polyurethane phase (X = 15.5 to 36.5% in polyurethane) and wide range of polyurethane (PU) to polyacrylate (PA) ratio (PU/PA = 20:80 to 80:20) were prepared, and the damping and mechanical properties of these materials were studied. The damping of polyurethane soft phase was increased and shifted to lower temperature with increased content of PA vitreous phase. The mechanical properties were improved with increasing PA contents. The results show that PA and the polyurethane hard segment interaction play a special role in chain interpenetration density and its magnitude is revealed by the decreased dispersed domain size observed by scanning electron microscopy (SEM) and increased loss area as measured by dynamic mechanical thermal analysis (DMTA). When the weight ratio of PU/PA was 40:60, the resulting SIN materials possessed better damping properties, independent of X concentration