The solution heat treatment (SHT) of the third generation of single crystal (SC) Ni-based superalloys required up to 45 h and was expensive. In this study, SHT based on liquid metal cooling (LMC) was optimized to greatly reduce processing time. The experimental and simulation results showed that residual segregation was evidently reduced, e.g., from 2.12 to 1.22 for the most heavily segregated Re. This led to a 16.7% increase in creep life, more uniform microstructures, and a decrease in solidification and homogenization porosity by a factor of 3.4. Structural refinement, approximately 0.32 times, served as the underlying mechanism for this optimization, which reduced diffusion distance and increased homogenization efficiency during SHT.