The present work demonstrates enhanced photocatalytic activity for zeolite-filled TiO2 nanotubes. ZSM-5 zeolite nanocrystals were grown on and into a TiO2 nanotubular skeleton (TiNT/ZSM-5) by multi-step hydrothermal synthesis consisting of in situ seeding and multiple in situ crystallization (MISC). The resulting zeolite nanocrystals were in the range of a few nanometers and they adhere well to the nanotubular inner walls. After crystallization, the photocatalytic activity of this zeolite-filled nanotube catalyst system was compared with neat anatase TiO2 nanotube (TiNT) and with calcined ZSM-5 powder. The results show for TiNT/ZSM-5 a highly enhanced efficiency for the decomposition of acetophenone (used as an aromatic model organic pollutant).