Neutron diffraction experiments can provide an extremely high-resolution structural picture of clay-fluid systems. Here we describe the application of time-of-flight neutron scattering to hydrated clays, including discussion of issues such as isotopic labelling, sample containment, and data analysis. Recent studies of hydrated vermiculites under ambient conditions are used as an example. We then describe a new high-pressure/high-temperature sample environment that is being used to study clay-fluid interactions, in situ under hydrostatic sedimentary basin conditions. This environment enables us to approximate conditions encountered during burial, at depths of up to 10 km.