<p>Structural metallic materials exposed to energetic particle bombardments often experience various types of irradiation-induced microstructural damage, thus degrading the mechanical properties of the materials in form of irradiation hardening and embrittlement. Nanostructured materials have shown better radiation resistance than their coarse-grained (CG) counterparts due to the existence of abundant defect sinks, such as grain boundaries, twin boundaries, and phase boundaries. However, recently developed nanocrystalline (NC) steels show limited room-temperature tensile ductility (< 1%), which may become a concern for their future application for nuclear reactors. The focus of this thesis is to explore the strength-ductility dilemma in modified 9Cr1Mo (T91) ferritic/martensitic (F/M) steel processed by thermomechanical treatment (TMT) and surface severe plastic deformation (SSPD) with an attempt to fabricate strong, ductile and radiation resistant F/M steels. </p> <p><b>Carbon partitioning</b> between the quenched martensite and the other phases (bainitic ferrite or retained austenite) is critical for enhancing the strength and ductility of T91 steel. The tensile properties of partially tempered (PT) T91 steel can be tailored through introducing bainitic ferrite with high-density nanoscale transition carbides and refined lath martensite. In addition, retained austenite was introduced by increasing the carbon concentration of T91 steel to 0.6 wt.%. The carbon-modified steel processed by quenching partitioning (Q-P) treatment exhibits an ultrahigh strength, ~ 2 GPa, with a uniform strain of ~ 5% due to the existence of coherent carbides, ultrafine martensite and retained austenite. </p> <p>Meanwhile, surface mechanical grinding treatment (SMGT) on T91 steel reveals that introducing <b>gradient structures</b> on the sample surface contributes to a higher strength and an improved plasticity than its homogeneously structured counterpart. The deformation mechanism of the gradient structures was investigated with the assistance of quasi <i>in situ</i> crystal orientation analyses. Furthermore, <i>ex situ</i> He ion irradiation on the gradient T91 steel indicates that radiation-induced damage, such as bubble-induced swelling and irradiation hardening, were gradually mitigated by grain refinement from the sample surface to the center, resulting in superior radiation resistance. The results obtained from this thesis may facilitate the design and fabrication of strong, ductile and radiation-tolerant F/M steels.</p>