The Pliocene, a geologic epoch spanning ~2.6-5.3 million years ago (Ma), was a period in Earth’s history where temperatures were several degrees warmer than today and atmospheric CO2 was close to modern levels, making it an analogue for future climate change. Following this interval, the planet’s climate shifted to the familiar glacial-interglacial cycles of the Pleistocene (~0-2.6 Ma), beginning with the development of extensive Northern Hemisphere ice sheets at ~2.7 Ma. In response to these changes through the Plio-Pleistocene, several components of the Earth System, particularly related to East Asia and the North Pacific Ocean, varied both temporally and spatially, further modifying regional and global climate through various feedbacks. In this thesis, I utilize a combination of geochemical proxies derived from North Pacific marine sediments as well as a regional climate model to better understand the evolution of the westerly winds, North Pacific Ocean circulation, and East Asian desert landscapes, across the last five million years. In Chapter 1, I reconstruct Pliocene dust fluxes at two different sites in the North Pacific using the constant flux proxy extraterrestrial 3He (3HeET), the first of such records in the Pliocene. Along with 3HeET-derived export productivity fluxes and sea surface temperatures from the westernmost core, I show that the Northern Hemisphere westerly winds, were shifted poleward and weaker during much of the warm Pliocene. Coinciding with the intensification of Northern Hemisphere Glaciation, the westerlies shifted equatorward and strengthened at ~2.7 Ma, and during subsequent glacial periods thereafter. Combining my dust flux record with others from different ocean basin, I find that these changes in the westerly winds were globally synchronous. Chapter 2, entitled “Pliocene Variability of Active Pacific Meridional Overturning Circulation: Reevaluating North Pacific Productivity and Redox Conditions from ~2.5-6 Ma”, presents additional 3HeET-based export productivity flux data, as well as redox element concentrations, from the central subarctic North Pacific through the Pliocene. The new records suggest elevated North Pacific export production during the interval spanning ~4-5.5 Ma, followed by a decrease in the mid-Pliocene (~3.5-4 Ma). Combining this new data with previously published records and modeling output, I provide additional evidence for an active Pacific meridional overturning circulation during the warmer-than-present Pliocene, and add constraints on its variability under various climatic conditions. In Chapter 3, I bring together two constant flux proxy-derived dust flux datasets from the same core in the western North Pacific Ocean to provide novel insight into Quaternary dust dynamics in East Asia. By utilizing constant flux proxies, and accounting for inputs of volcanic material, I show for the first time that dust input to the North Pacific decreased over the last ~2.7 Myr, particularly during glacial periods. While quite different from other previously published dust datasets, this finding is consistent with our current understanding of East Asian dust production mechanisms, and acts as a strong impetus to perform more comprehensive studies of dust fluxes to the North Pacific and other depositional areas downwind of arid regions. Chapter 4 transitions to a terrestrial setting, in which I investigate the impacts of shifting arid region surface albedo on the atmospheric boundary layer using the Hami Basin, China, as a test location. Combining new simulations from the Weather Research and Forecasting base model and available geologic data, I report a previously undescribed “wind-albedo-wind” feedback process. Specifically, I propose that wind erosion, in conjunction with surficial sediments of various albedos, leads to altered wind speeds, and eventually fluctuations in erosion itself. In Chapter 5, I expand upon the work in the preceding chapter by coupling the Weather Research and Forecasting model with a chemistry component to simulate dust emissions. In addition, along with albedo, I characterize previously interpreted surface changes through time to reflect shifts in erodibility and surface roughness. I conclude that although albedo does ultimately influence near-surface wind speeds and dust emissions as predicted in my earlier study, the effects of variable surface roughness and erodibility dominate. Integrating these results with an updated interpretation of the geologic evolution of the Hami Basin, we find that during various periods of the last ~700 ky, the Hami Basin, and likely the greater stony Gobi Desert, could have been much more important dust sources than today.