Abstract: The Nalinggou–Daying uranium metallogenic belt is situated at the northern Ordos Basin, China. Petrographical, mineralogical and geochemical techniques were used to study the ore-bearing sandstones and host rocks in the Nalinggou–Daying uranium metallogenic belt. The present study shows that uranium minerals, i.e., coffinite, pitchblende, and brannerite, are mostly disseminated around pyrite and detrital particles. The ore-bearing sandstones are enriched in organic matter, with which this reductive environment influenced uranium leaching. The carbonate concentration of the uranium ores is markedly higher than that of the host rocks, and intense carbonatization occurs in the ore-bearing sandstones. In this case, the usage of the classical in-situ leach uranium mining technique by injecting H2SO4 + H2O2 solution produces calcium sulfate precipitate, which can lead to blocking of the ore-bearing strata. For this reason, laboratory and field uranium mining tests were conducted using CO2 + O2 in-situ leaching technology and were demonstrated to be successful, illustrating that this approach is technically feasible. Inhibiting ore bed blockage and increasing the amount of injected O2 are important for uranium leaching in this setting.