A novel microgravimetric immunosensor has been developed using TiO2 nanoparticle-modified immunoassay and silver enhancement reaction. An antibody-conjugated TiO2 nanoparticle is bound to the AFP antigen immobilized on a quartz resonator. When the nanoparticles are exposed to UV light in a silver nitrate solution, the photocatalytic reduction of silver ions results in the formation of metallic silver onto the nanoparticles and induces a decrease in the resonance frequency. The frequency change by this photocatalytic reduction reaction is three orders of magnitude larger than the change by antigen binding alone. The efficiency of the photocatalytic reaction has been found to increase with the fraction of anatase crystallites in the nanoparticles and the concentration of the AgNO3 solution. The results highlight the potential of the photocatalytic nanoparticles for the detection of low concentrations of target molecules using gravimetric sensors.