We present experimental results on the performance of a series of coated, D-shaped optical fibre sensors that display high spectral sensitivities to external refractive index. Sensitivity to the chosen index regime and coupling of the fiber core mode to the surface plasmon resonance (SPR) is enhanced by using specific materials as part of a multi-layered coating. We present strong evidence that this effect is enhanced by post ultra-violet radiation of the lamellar coating that results in the formation of a nano-scale surface relief corrugation structure, which generates an index perturbation within the fibre core that in turn enhances the coupling. We have found reasonable agreement when modelling the fibre devices. It was found that the SPR devices operate in air with high coupling efficiency in excess of 40dB with spectral sensitivities that outperform a typical long period grating, with one device yielding a wavelength spectral sensitivity of 12000nm/RIU in the important aqueous index regime. The devices generate surface plasmon resonances over a very large wavelength range; (visible to 2m) by alternating the polarisation state of the illuminating light.