Given the rapid nature of climate change occurring in the Arctic and the difficulty climate models have in quantitatively reproducing observed changes such as sea ice loss, it is important to improve understanding of the processes leading to climate change in this region, including the role of short-lived climate pollutants such as aerosols and ozone. It has long been known that pollution produced from emissions at midlatitudes can be transported to the Arctic, resulting in a winter/spring aerosol maximum known as Arctic haze. However, many uncertainties remain about the composition and origin of Arctic pollution throughout the troposphere; for example, many climate–chemistry models fail to reproduce the strong seasonality of aerosol abundance observed at Arctic surface sites, the origin and deposition mechanisms of black carbon (soot) particles that darken the snow and ice surface in the Arctic is poorly understood, and chemical processes controlling the abundance of tropospheric ozone are not well quantified. The International Polar Year (IPY) Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, Climate, Chemistry, Aerosols and Transport (POLARCAT) core project had the goal to improve understanding about the origins of pollutants transported to the Arctic; to detail the chemical composition, optical properties, and climate forcing potential of Arctic aerosols; to evaluate the processes governing tropospheric ozone; and to quantify the role of boreal forest fires. This article provides a review of the many results now available based on analysis of data collected during the POLARCAT aircraft-, ship-, and ground-based field campaigns in spring and summer 2008. Major findings are highlighted and areas requiring further investigation are discussed.