Optical fiber gratings (OFGs), especially long‐period gratings (LPGs) and etched or tilted fiber Bragg gratings (FBGs), are playing an increasing role in the chemical and biochemical sensing based on the measurement of a surface refractive index (RI) change through a label‐free configuration. In these devices, the electric field evanescent wave at the fiber/surrounding medium interface changes its optical properties (i.e. intensity and wavelength) as a result of the RI variation due to the interaction between a biological recognition layer deposited over the fiber and the analyte under investigation. The use of OFG‐based technology platforms takes the advantages of optical fiber peculiarities, which are hardly offered by the other sensing systems, such as compactness, lightness, high compatibility with optoelectronic devices (both sources and detectors), and multiplexing and remote measurement capability as the signal is spectrally modulated. During the last decade, the growing request in practical applications pushed the technology behind the OFG‐based sensors over its limits by means of the deposition of thin film overlays, nanocoatings, and nanostructures, in general. Here, we review efforts toward utilizing these nanomaterials as coatings for high‐performance and low‐detection limit devices. Moreover, we review the recent development in OFG‐based biosensing and identify some of the key challenges for practical applications. While high‐performance metrics are starting to be achieved experimentally, there are still open questions pertaining to an effective and reliable detection of small molecules, possibly up to single molecule, sensing in vivo and multi‐target detection using OFG‐based technology platforms.