The elimination of organic molecules from wastewater is required to prevent harm to aquatic creatures. In the past, it has been demonstrated that zeolite-based systems provide excellent prospects for wastewater treatment; nonetheless, the majority of zeolite systems documented to date suffer from sinking in water and a saturated adsorption site. In the present work, we endeavored to create zeolite-based composite systems with excellent floatability, adsorption capacity, and photocatalytic activity. Furthermore, we verified that these composites could be easily removed from the treated water. Consequently, a tri-layer floating photocatalyst/adsorbent was created by deposition of silicalite-1, a pure silica MFI-type zeolite (PSZ), and TiO₂ on hollow glass microspheres (HGMs). To create floating adsorbents, a thin coating of silicalite-1 was crystallized on the thick walls of HGMs (PSZHGMs). Using the sol-gel technique, a layer of TiO₂ was placed on PSZ-HGM surfaces to create photocatalytic composites (TiO2/PSZ-HGMs). By introducing HGMs to an alkali solution comprising tetrapropylammonium hydroxide and tetraethyl orthosilicate, followed by hydrothermal synthesis at 180°C for 40 hours, excellent PSZ coverage, and attachment were obtained on HGM surfaces. TiO₂ could cover the PSZ surface uniformly without blocking the zeolite pores during subsequent deposition. Using methylene blue, the wastewater treatment capacity of the synthesized materials was determined (MB). TiO2/PSZ-HGMs, which displayed both photocatalytic and adsorption capabilities, operated synergistically with UV-C irradiation to decrease MB content by 98% in 2 h. Consequently, these materials may have considerable promise in wastewater treatment operations.