Microstructure models seek to explain or predict various material properties in terms of the structure or chemical composition at scales of several hundred nanometres to several hundred micrometres. Such models therefore bridge the scaling gap between atomistic models and continuum methods, and consequently can help establish and validate scaling relations across those scales. Microstructure models have been applied to cementitious materials for at least four decades to help understand setting, strength development, rheological properties, mechanical behavior, and transport properties. This letter describes the current state of cement microstructure modelling in several areas that are important for engineering. It is not meant to be an exhaustive review, instead highlighting the kinds of models that can now be applied to different aspects of cement binder behaviour. Special attention is paid to challenges or limitations of each kind of model. This is done to promote the judicious use and interpretation of models and especially to indicate where future research could make inroads on problems that are currently inaccessible to microstructure models.