Barium titanate/nitrile butadiene rubber (BT/NBR) and polyurethane (PU) foam were combined to prepare a sound-absorbing material with an alternating multilayered structure. The effects of the cell size of PU foam and the alternating unit number on the sound absorption property of the material were investigated. The results show that the sound absorption efficiency at a low frequency increased when decreasing the cell size of PU foam layer. With the increasing of the alternating unit number, the material shows the sound absorption effect in a wider bandwidth of frequency. The BT/NBR-PU foam composites with alternating multilayered structure have an excellent sound absorption property at low frequency due to the organic combination of airflow resistivity, resonance absorption, and interface dissipation.