Ferritic/martensitic (FM) steels such as HT-9, T-91 and NF12 with chromium concentrations in the range of 9-12 at.% Cr and high Cr ferritic steels (oxide dispersion strengthened steels with 12-18% Cr) are receiving increasing attention for advanced nuclear applications, e.g. cladding and duct materials for sodium fast reactors, pressure vessels in Generation IV reactors and first wall structures in fusion reactors, thanks to their advantages over austenitic alloys. Predicting the behavior of these alloys under radiation is an essential step towards the use of these alloys. Several radiation-induced phenomena need to be taken into account, including phase separation, solute clustering, and radiation-induced segregation or depletion (RIS) to point defect sinks. RIS at grain boundaries has raised significant interest because of its role in irradiation assisted stress corrosion cracking (IASCC) and corrosion of structural materials. Numerous observations of RIS have been reported on austenitic stainless steels where it is generally found that Cr depletes at grain boundaries, consistently with Cr atoms being oversized in the fcc Fe matrix. While FM and ferritic steels are also subject to RIS at grain boundaries, unlike austenitic steels, the behavior of Cr is less clear with significant scatter and no clear dependency on irradiation condition or alloy type. In addition to the lack of conclusive experimental evidence regarding RIS in F-M alloys, there have been relatively few efforts at modeling RIS behavior in these alloys. The need for predictability of materials behavior and mitigation routes for IASCC requires elucidating the origin of the variable Cr behavior. A systematic detailed high-resolution structural and chemical characterization approach was applied to ion-implanted and neutron-irradiated model Fe-Cr alloys containing from 3 to 18 at.% Cr. Atom probe tomography analyses of the microstructures revealed slight Cr clustering and segregation to dislocations and grain boundaries in the ion-irradiated alloys. More significant segregation was observed in the neutron irradiated alloys. For the more concentrated alloys, irradiation did not affect existing Cr segregation to grain boundaries and segregation to dislocation loops was not observed perhaps due to a change in the dislocation loop structure with increasing Cr concentration. Precipitation of [alpha]' was observed in the neutron irradiated alloys containing over 9 at.% Cr. However ion irradiation appears to suppress the precipitation process. Initial low dose ion irradiation experiments strongly suggest a cascade recoil effect. The systematic analysis of grain boundary orientation on Cr segregation was significantly challenged by carbon contamination during ion irradiation or by existing carbon and therefore carbide formation at grain boundaries (sensitization). The combination of the proposed systematic experimental approach with atomistic modeling of diffusion processes directly addresses the programmatic need for developing and benchmarking predictive models for material degradation taking into account atomistic kinetics parameters.