A novel visible light-driven photocatalyst film, MoS2/Ag/TiO2, was synthesized on a glass-fiber membrane. The composite catalyst film had a multi-layer structure with Ag as nanoconjunctions between the MoS2 and TiO2 layers. The catalyst film performed well for both photocatalytic hydrogen production and organic degradation in a two-chamber photo-reactor under either solar or visible light. Hydrogen was produced in the cathode side chamber while the model organic was decomposed in the anode side chamber. The specific hydrogen production rate went through a maximum of 85 mmol/m2-h with an energy conversion efficiency of 0.85%, while the maximum specific organic carbon removal for formic acid under solar light reached 1,520 mg/m2-h. It is apparent that Ag between the TiO2 and MoS2 layers allowed the transfer of photo-excited electrons via TiO2 → Ag → MoS2 for organic degradation and H+ reduction (e.g. hydrogen evolution) in two different chambers.