Piezoelectric nanomaterials have been utilized to realize effective charge separation for degrading organic pollutants in water under the action of mechanical vibrations. However, in particulate form, the nanostructured piezoelectric catalysts can flow into the aqueous pollutant and limit its recyclability and reuse. Here, we report a new method of using a barium titanate (BaTiO3, BTO)-polydimethylsiloxane composite porous foam catalyst to address the challenge of secondary pollution and reusable limits. Piezo-catalytic dye degradation activity of the porous foam can degrade a Rhodamine B (RhB) dye solution by similar to 94%, and the composite material exhibits excellent stability after repeated decomposition of 12 cycles. It is suggested that under ultrasonic vibrations, the piezoelectric BTO materials create separated electron-hole pairs that react with hydroxyl ions and oxygen molecules to generate superoxide (O-center dot(2)-) and hydroxyl ((OH)-O-center dot) radicals for organic dye degradation. The degradation efficiency of RhB is associated with the piezoelectric constant, the specific surface area, and the shape of the material.