This paper is a keynote presentation from the 13th International Congress on the Chemistry of Cement. It discusses the underlying principles of hydration and recent evidence for the mechanisms governing this process in both Portland cements and other cementitious materials. Given the overriding imperative to improve the sustainability of cementitious materials, routes to reducing CO2 emissions are discussed and the impact of supplementary materials on hydration considered. (C) 2011 Elsevier Ltd. All rights reserved.