In the present study, X-ray diffraction, electron probe microanalysis, and transmission electron microscopy, among other advanced characterization methods, were used to analyze the microstructure and mechanical properties of the 9Ni steel treated at different heat treatment conditions. The goal was to reveal the dual-optimal strengthening mechanism of “low yield ratio and ultra-cryogenic toughness” of the investigated steel. The experimental results indicated that the 9Ni steel, designed with a ''Ni–Cr–Mo'' multi-elemental composition, balanced its hardenability and corrosion resistance. After the Q-Q' (710 °C) -T process, the diffusion of Cr and Mo atoms in the steel accelerated, while the Fe displacement diffusion formed a more stable FeNi face-centered cubic structure with a lattice energy of −76.98 eV. At this stage, the microstructure of the investigated steel primarily consisted of tempered sorbite (with an average effective grain size of 13.1 μm), tempered martensite lath clusters, reversed austenite, and precipitated Cr23C6 and Mo2C particles. This composition resulted in a low yield ratio. The concentration of Ni near the lath clusters promoted the formation of the reversed austenite with a volume fraction of 10.2%, ensuring the cryogenic toughness of the investigated steel.