This study aimed to investigate the impact of hydrogen content, up to 1217 ppm, on the mechanical properties of Zircaloy-4, with a particular focus on the formation and impact of hydrides. Tensile specimens were tested across a range of temperatures and hydrogen concentrations. The results revealed a pronounced ductile-to-brittle transition associated with hydride formation. When the hydrogen content in the specimens ranged between 700 and 850 ppm, a ductile-to-brittle transition was observed at temperatures of 25 °C, 50 °C, and 75 °C. At 25 °C, the ultimate tensile strength (UTS) of Zircaloy-4 linearly increased as the hydrogen concentration rose from 0 to 1217 ppm H. However, at higher temperatures, the behavior of UTS became more complex, especially in the hydrogen concentration ranges of 500–850 ppm H. Elongation (EL) in the hydrided specimens was affected by both temperature and hydrogen concentration. As hydrogen concentration increased, there was a noticeable decline in uniform EL, while non-uniform EL showed even more significant reductions. Scanning electron microscopy (SEM) analysis of the fracture surfaces revealed that quasi-cleavage features became evident when the hydrogen content reached 850 ppm H, across all tested temperatures. These findings not only provide a quantitative assessment of the safety implications of Zircaloy-4 in nuclear reactor applications but also highlight the importance of the hydrogen charging process and mechanical testing in understanding its mechanical behavior.