This article is to summarize the process development and key characterization results for the newly-developed Fe-9Cr based nanostructured ferritic alloys (NFAs) with high fracture toughness. One of the major drawbacks from pursuing ultra-high strength in the past development of NFAs is poor fracture toughness at high temperatures although a high fracture toughness is essential to prevent cracking during manufacturing and to mitigate or delay irradiation-induced embrittlement in irradiation environments. A study on fracture mechanism using the NFA 14YWT found that the low-energy grain boundary decohesion in fracture process at a high temperature (>200 °C) resulted in low fracture toughness. Lately, efforts have been devoted to explore an integrated process to enhance grain bonding. Two base materials were produced through mechanical milling and hot extrusion and designated as 9YWTV-PM1 and 9YWTV-PM2. Isothermal annealing (IA) and controlled rolling (CR) treatments in two phase region were used to enhance diffusion across the interfaces and boundaries. The PM2 alloy after CR treatments showed high fracture toughness (KJQ) at represented temperatures: 240-280 MPa √m at room temperature and 160-220 MPa √m at 500 °C, which indicates that the goal of 100 MPa √m over possible nuclear application temperature range has been well achieved. Furthermore, it is also confirmed by comparison that the CR treatments on 9YWTV-PM2 result in high fracture toughness similar to or higher than those of the conventional ferritic-martensitic steels such as HT9 and NF616.