This study investigates the role of grain-boundary precipitates in enhancing creep rupture strength of Ni-based alloys through analysis of Ni-15Cr-15Mo and Ni-15Cr-17Mo (at.%) model alloys. The investigation focused on the “Grain-boundary Precipitation Strengthening (GBPS)” effect from the thermally stable TCP phase, a phenomenon previously observed in Fe-Cr-Ni-Nb austenitic heat-resistant steels. Through multi-step heat treatments, specimens were prepared with varying grain boundary coverage ratios (ρ) of TCP P phase (oP56) and consistent grain-interior hardness from GCP Ni2(Cr, Mo) phase (oP6). In the 15 at.% Mo alloy, specimens with a higher coverage ratio (~80%) demonstrated significantly improved creep performance, achieving nearly four times longer rupture time (3793 h vs. 1090 h) at 300 MPa and 973 K compared to specimens with lower coverage (~35%). However, the 17 at.% Mo alloy showed unexpectedly lower performance despite high coverage ratios, attributed to preferential cavity formation at bare grain boundaries. These findings confirm that GBPS via thermally stable TCP phase effectively enhances creep properties in Ni-based alloys, with grain boundary coverage ratio being more crucial than intragranular precipitation density.