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The growth of atheism and other forms of ‘unbelief’ in many parts of the world is attracting increasingly wide attention. Yet significant questions remain about how to understand such phenomena, and scientists rely still on categories developed by social actors, not social scientists, to do so. The term ‘atheism’ has its origins in ancient Greece and has been applied to a wide array of phenomena including a lack of devotion to Roman deities and a lack of belief in all supernatural agencies; and ‘unbelief’ derives from Western and Christian traditions and indicates the absence of belief in God(s), and sometimes the absence of belief in other supernatural forces and the afterlife. If we are to advance our scientific understanding in these areas, we need to account for the diverse psychological and social phenomena and processes subsumed under these terms. We do not currently know how best to characterize the various forms of unbelief as psychological and sociological phenomena, the extent to which other beliefs – about religion, or the existential – underpin these forms, how diverse they are, and how they vary across demographic groups and cultures. Yet understanding the nature and variety of unbelief is necessary if we are, in future, to answer big questions about the causes of ‘unbelief’ and its effects on such outcomes as personal wellbeing and social cohesion. The Understanding Unbelief project will be the first major scientific research program to address the nature and variety of unbelief. It includes (i) grant competitions to generate multidisciplinary research into diverse forms of unbelief across demographic groups and cultural settings, and (ii) core interdisciplinary research working across these forms, groups, and settings to build a more integrated understanding of unbelief. Together these strategies will produce the first scientifically coherent account of unbelief and of what it means to be an unbeliever.