The reactor pressure vessel (RPV) is a critical barrier in nuclear power plants, but its embrittlement during service poses a significant safety challenge. This study investigated the effects of Cu-enriched clusters on the mechanical and magnetic properties of Fe-0.9 wt.%Cu model alloys through thermal aging. Using Vickers hardness tests, Magnetic Barkhausen Noise (MBN) detection, and Atom Probe Tomography (APT), the study aimed to establish a quantitative correlation between MBN signals, Vickers hardness, and Cu-enriched clusters, facilitating the non-destructive testing of RPV embrittlement. Experimental results showed that the hardness and MBN parameters (RMS and Vpp values) changed significantly with aging time. The hardness increased rapidly in the early stage (under-aged), followed by a plateau and then a decreasing trend (over-aged). In contrast, MBN parameters decreased initially and then increased. APT analysis revealed that Cu-enriched clusters increase in size to 4.60 nm and coalesced during aging, with their number density peaking to 3.76 × 1023 m−3 before declining. An inverse linear correlation was found between MBN signals and the combined factor Nd2Rg (product of the number density squared and the mean radius of Cu-enriched clusters). This correlation was consistent across both under-aged and over-aged states, suggesting that MBN signals can serve as applicable indicators for the non-destructive evaluation of RPV steel embrittlement.