We have been using the technique of pulsed neutron powder diffraction to study several problems in the physics and chemistry of the actinide elements. In these elements one often encounters very complex structures resulting from polymorphic transformations presumably induced by the presence of 5f-electrons. For exampie, at least five distinct structures of plutonium metal are found between room temperature and its melting point of 640°C, and two of the structures are monoclinic! Single crystals are usually not available, and the high resolution which is intrinsic to the time-of-flight powder technique is a powerful tool in the solution of complex structural problems. The relatively low absorption coefficients for neutrons for at least some actinide isotopes is an advantage when surface oxidation is a problem (as in high-temperature experiments) and provides good particle statistics so that high-quality data are available for Rietveld refinement. The low absorption of neutrons by other materials such as vanadium and fused silica enables the use of these materials for the containment of samples in high- and low-temperature environments, and the fixed geometry of the time-of-flight technique simplifies the design of furnaces and cryostats.