Microbubble fabrication of poly(dimethylsiloxane) (PDMS) beads with incorporated TiO2 provides a low-density, microstructured photocatalyst that is buoyant in water. This approach surmounts many of the challenges traditionally encountered in the generation of buoyant photocatalysts, an area which is critical for the implementation of widespread environmental cleaning of organic pollutants in water resources. Because the incorporation into the polymer bead surface is done at low temperatures, the crystal structure of TiO2 is unaltered, ensuring high-quality photocatalytic activity, while PDMS is well-established as biocompatible, temperature stable, and simple to produce. The photocatalyst is shown to degrade methylene blue faster than other buoyant, TiO2-based photocatalysts, and only an order of magnitude less than direct suspension of an equivalent amount of photocatalyst in solution, even though the photocatalyst is only present at the surface of the solution. The reusability of the TiO2/PDMS beads is also strong, showing no depreciation in photocatalytic activity after five consecutive degradation trials.