There remains substantial debate concerning the relative roles of tectonics and global climate in driving the evolution of climate in Central Asia. Today, interior Asia—including the Taklamakan, Gobi, and Ordos Deserts—is exceptionally arid and is surrounded by distinct rainfall boundaries, such as those generated by the Asian monsoon systems to the east and south and those generated by high topography to the north and west. Determining how and why these boundaries have varied over the Neogene is hindered by the lack of a single proxy that can be broadly applied through space and time. We construct isoscapes of pedogenic carbonate δ13C (δ13Cc) over the Neogene in Asia by combining a compilation of 2236 published measurements with new data from three localities in northern Central Asia. Pedogenic carbonate δ13C records local aridity—excepting localities impacted by C4 grasslands and during large changes in atmospheric pCO2—through variations in soil respiration, depth of carbonate formation, and the effect of water stress on plant δ13C. Together, these effects reflect changes in both primary productivity and mean annual precipitation. Throughout the Neogene, we find consistent and exceptionally high δ13Cc in interior Asia with a ring of lower δ13Cc that demarcates higher precipitation. This persistent ring of lower δ13Cc corresponds in the south and east with the influence of the Asian monsoon systems; in the west and north, it reflects both orographic rainfall due to uplift of the Tian Shan and to moisture delivery by the mid-latitude westerlies. Finally, δ13Cc and, hence, aridity increases regionally in the latest Neogene, reflecting the effects of Northern Hemisphere glaciation and cooling. This widespread “de-greening” would have increased regional albedo and modified basin-scale water balances, resulting in greater dust fluxes due to reduced vegetative cover and precipitation.