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Due to its excellent properties, polydimethylsiloxane (PDMS) foam has recently attracted significant academic and industrial attention. In this study, a facile and green method was developed for PDMS foam synthesis. The PDMS foam was prepared by using the gas foaming method with eco-friendly materials, namely NaHCO₃ as a blowing agent and acetic acid as the catalyst. By changing the ratios of the reactants and the curing temperature, foams with varying properties were obtained. The water contact angle of the obtained PDMS foams ranged from 110° to 139°. We found that the PDMS foams can be compressed to a maximum strain of 95% and retain their original size, showing excellent mechanical properties. The synthesized PDMS foams were tested as an absorbent to remove benzene, toluene, and xylene (BTX) from the water. It exhibited good selectivity, outstanding reusability, and absorption capacity. Its capability to remove a large amount of organic solvent from the water surface suggests the great promise of PDMS foam in recovering spilled organic compounds from water, with excellent separation performance for continuous treatment.