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Background Under-five mortality is declining in Ghana and many other countries. Very few studies have measured under-five mortality—and its social and environmental risk factors—at fine spatial resolutions, which is relevant for policy purposes. Our aim was to estimate under-five mortality and its social and environmental risk factors at the district level in Ghana. Methods and Findings We used 10% random samples of Ghana’s 2000 and 2010 National Population and Housing Censuses. We applied indirect demographic methods and a Bayesian spatial model to the information on total number of children ever born and children surviving to estimate under-five mortality (probability of dying by 5 y of age, 5q0) for each of Ghana’s 110 districts. We also used the census data to estimate the distributions of households or persons in each district in terms of fuel used for cooking, sanitation facility, drinking water source, and parental education. Median district 5q0 declined from 99 deaths per 1,000 live births in 2000 to 70 in 2010. The decline ranged from 40% in southern districts, where it had been lower in 2000, exacerbating existing inequalities. Primary education increased in men and women, and more households had access to improved water and sanitation and cleaner cooking fuels. Higher use of liquefied petroleum gas for cooking was associated with lower 5q0 in multivariate analysis. Conclusions Under-five mortality has declined in all of Ghana’s districts, but the cross-district inequality in mortality has increased. There is a need for additional data, including on healthcare, and additional environmental and socioeconomic measurements, to understand the reasons for the variations in mortality levels and trends., In a census-based study, Majid Ezzati and colleagues use demographic modeling to estimate district-level variation in under-five mortality across Ghana., Author Summary Why Was This Study Done? Deaths among children younger than five years old have been declining worldwide for the past few decades. Children’s death rates in sub-Saharan Africa, although also declining, remain higher than in other regions. Ghana has performed better than most other sub-Saharan African countries in terms of reducing child deaths, but we lack information on how much child mortality varies in different parts of Ghana. Also, it is not known how factors such as low education of mothers or not having clean water or improved toilet facilities that increase the risk of illness and death among children vary in different parts of Ghana. The purpose of our study was to provide information on changes in the child death rate, and the social and environmental factors associated with it, for all of Ghana’s 110 districts between the years 2000 and 2010. What Did the Researchers Do and Find? Information from two national censuses in 2000 and 2010 and sophisticated statistical models were used to make estimates of the child death rate in each district for the years 2000 and 2010 and for change between these two years. The risk of children dying before they reach age five was higher in northern Ghana than it was in the southern part of the country. Child death rates went down in every district in Ghana between 2000 and 2010, but progress was slower in northern Ghana than in the southern part of the country. More women and men in the country had completed primary school education in 2010 than in 2000, and more homes had access to clean water and improved toilet facilities and cleaner cooking fuels like liquefied petroleum gas. Use of liquefied petroleum gas for cooking may reduce the risk of child death in Ghana. What Do These Findings Mean? There should be strategies to help districts where young children are at a relatively higher risk of dying, largely those in northern Ghana, to catch up with those districts with lower child mortality. Some of the actions needed may be related to social and environmental factors like education, clean sanitation, and cooking fuels. But it is likely that there is an important role for healthcare, which was not investigated in this study. It is important for Ghana and other sub-Saharan African countries to improve the measurement and monitoring of child mortality and its social, environmental, and healthcare risk factors at the community level.