The extent and level of solute segregation to individual dislocations may be quantified by atom probe tomography. The technique is best applied to materials with high dislocation densities, such as cold worked, mechanically alloyed, or neutron-irradiated materials. Dislocations may be observed in field ion images by a change of the normal concentric atom terraces at crystallographic poles to spirals. Solute segregation is evident in field ion images by brightly imaging atoms near the core of the dislocation. Dislocations are evident in atom maps in the three-dimensional atom probe by linear regions of enhanced solute concentration. The maximum separation envelope and tracer methods may be used to quantify the levels of solute at the dislocation at the subnanometer scale. Examples of interstitial and substitutional element segregation in a mechanically alloyed, oxide dispersion strengthened ferrite steel and phosphorus segregation to dislocations in neutron-irradiated pressure vessel steels are presented.