Ionic self-assembled multilayers deposited on long period fiber gratings (LPGs) yield dramatic resonant-wavelength shifts, even with nanometer-thick films. Fine control of the refractive index and the thickness of these films was achieved by altering the relative fraction of the anionic and cationic materials combined with layer-by-layer deposition. We demonstrate the feasibility of this highly controllable deposition technique for fine-tuning grating properties. In addition a variety of biological and chemical sensing agents can easily be incorporated into these films, which makes this an attractive platform for realization of high-performance LPG-based sensors.