Accurate, cost-efficient, and safe hydrogen sensors will play a key role in the future hydrogen economy. Optical hydrogen sensors based on metal hydrides are attractive owing to their small size and costs and the fact that they are intrinsically safe. These sensors rely on suitable sensing materials, of which the optical properties change when they absorb hydrogen if they are in contact with a hydrogen-containing environment. Here, we illustrate how we can use alloying to tune the properties of hydrogen-sensing materials by considering thin films consisting of tantalum doped with ruthenium. Using a combination of optical transmission measurements, ex situ and in situ X-ray diffraction, and neutron and X-ray reflectometry, we show that introducing Ru in Ta results in a solid solution of Ta and Ru up to at least 30% Ru. The alloying has two major effects: the compression of the unit cell with increasing Ru doping modifies the enthalpy of hydrogenation and thereby shifts the pressure window in which the material absorbs hydrogen to higher hydrogen concentrations, and it reduces the amount of hydrogen absorbed by the material. This allows one to tune the pressure/concentration window of the sensor and its sensitivity and makes Ta_1-yRu_y an ideal hysteresis-free tunable hydrogen-sensing material with a sensing range of >7 orders of magnitude in pressure. In a more general perspective, these results demonstrate that one can rationally tune the properties of metal hydride optical hydrogen-sensing layers by appropriate alloying.