Hydrogen is a cornerstone of the emerging net-zero carbon economy, and its widespread deployment demands sensitive, stable, and scalable detection technologies. In this study, we present a comparative performance analysis of Fibre Bragg Grating (FBG) sensors coated with nanometre-thick metal hydride-forming layers—tantalum (Ta), tantalum-palladium alloy (Ta_0.88 Pd_0.12), palladium (Pd), and palladium-gold alloy (Pd _0.6 Au_0.4)—for optical hydrogen sensing. The integration of Ta and Ta _0.88 Pd_0.12, two tantalum-based metal hydrides, with FBG sensors is introduced here for the first time, offering a promising alternative to conventional Pd-based materials. All coatings were deposited via magnetron sputtering and tested under controlled hydrogen exposure across concentrations ranging from 0.001% to 100% H₂. The Ta-based FBGs exhibited outstanding performance, showing a remarkably linear relative wavelength shift over the full tested range (0.001% to 100% H₂), with sensitivity detectable down to 10 ppm—the lowest concentration achievable in the current setup. Both Ta and Ta_0.88 Pd_0.12 sensors exhibited fully reversible and hysteresis-free response characteristics, with rapid response and recovery. Among them, the Ta_0.88 Pd_0.12 sensor with a 100 nm coating demonstrated the highest logarithmic sensitivity of ∼9 pm/decade(%H₂), corresponding to a 9 pm wavelength shift for every tenfold increase in hydrogen concentration between 0.001% and 100% H₂. In contrast, Pd and Pd _0.6 Au_0.4 sensors showed degraded performance at low concentrations and greater signal hysteresis. These results underscore the potential of Ta and Ta _0.88 Pd_0.12 coatings as robust and high-performance alternatives to conventional Pd-based materials for next-generation distributed fibre-optic hydrogen sensing systems.