In this study, a polymer-based two-dimensional photonic crystal (PhC) cavity for visible-light-based optical-sensing applications was designed and fabricated for the first time. The PhC cavity configuration was designed to operate at 650 nm, and fabricated with a polymer (resist) on a silicon substrate using electron-beam lithography. For investigating sensing applications based on shifting of condition exhibiting a photonic bandgap (PBG), the polymer monolayer deposition (layer-by-layer method) was monitored as the light-intensity change at the cavity position. Consequently, the monolayer-level detection of polyions was achieved.