In this work, we have studied the suitability of graphene oxide-based thin films to be not only excellent sensitive coatings but also lossy mode resonance (LMR)-generating materials. Thin films of graphene oxide (GO) and polyethylenimine (PEI) fabricated by means of layer-by-layer assembly were selected in this study. Two optical fiber devices with 8 and 20 bilayers of the LMR-generating coating were fabricated and characterized as refractometers. Both devices show no hysteresis and high sensitivity, improving previously reported values. This research opens very promising and exciting possibilities in the field of optical fiber sensors based on LMR, strategically including specific recognition groups to the device surface to exploit this high sensitivity for monitoring a range of target analytes. The carboxylate functional groups at the edges of the GO sheets should provide excellent attachment sites for the required coupling chemistry to realize such devices.