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A relative humidity sensor based on the deposition of electrostatic self-assembled alumina ( Al2O3) and poly(sodium 4-styrenesulfonate) on the cladding of a long-period fiber grating (LPFG) has been designed. The sensitive material has a lower refractive index than that of the fiber cladding, which limits the sensitivity of the LPFG response. In order to enhance its sensitivity, a previous high refractive index coating has been deposited. The overlay thickness is of the order of magnitude of the light wavelength used to interrogate the sensor. A theoretical model of multilayer cylindrical waveguides based on coupled-mode theory has been used to predict the phenomenon. Experimentally, an increased wavelength shift of the attenuation bands (75%) was obtained during the fabrication of the sensor, and, what is more important, the sensitivity was improved by a ratio of almost four. The proposed method improves the performance of LPFG-based sensors characterized by overlays of low refractive index.