The development of Hydrogen Internal Combustion Engine (H2-ICEs) to replace conventional fuel engines is expected to be an effective way to reduce CO2 emissions, but some NOx emitted from the H2-ICEs still should be eliminated by the selective catalytic reduction of NOx with H2 (H2-SCR). Large amount of platinum oxide existed on Pt/TiO2 leads to its low H2-SCR activity. In contrast, the Zr-modified Pt/TiO2 catalysts exhibit a higher NOx conversion and N2 selectivity in a wider temperature window (100–180 °C) than those of Pt/TiO2. The appropriately weakened strong interaction between Pt and TiO2 by Zr induces more Pt0 species, which are active sites for the activation of NOx and H2 in H2-SCR reaction. More oxygen vacancies caused by the formation of Zr-Ov-Ti3+ bands involve in the activation of NOx and the adsorption of nitrates (NOx−) species. Furthermore, in situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTs) demonstrates that Pt/ZrxTi1-x catalysts possess more adsorbed NOx− species and a faster reduction rate for them. Monodentate and bridged nitrates are considered to be more reactive with H2 than bidentate nitrates at relatively low temperatures. This work provides directions for the development of high-performance H2-SCR catalysts and the modulation of the conversion temperature.