Abstract Highly sensitive long-period fiber gratings (LPFG) was developed for label-free and rapid detection of Staphylococcus aureus (S. aureus). Specifically, the LPFG was functionalized with antibody and nanopitted polyelectrolyte coatings to facilitate bacterial adhesion and thus enhance the sensitivity of bacteria detection. The kinetics of S. aureus adhesion on functional coatings were tracked by surface morphology evolution and time-resolved resonance wavelength shift of the coated LPFG at a flow rate of 30 μl/ml and 37 °C in the concentration range of 104–108 colony forming unit (CFU)/ml. S. aureus detection at concentrations as low as 224 CFU/ml can be achieved within a short time span of 30 min. The LPFG-based biosensor can be readily adapted to a variety of biophotonic platforms, for applications such as food safety inspection, environmental monitoring, clinical diagnostics, and medical applications.