The effects of micro-additions of boron and zirconium on grain-boundary (GB) structure and strength in polycrystalline γ(f.c.c.) plus γ'(L12) strengthened Co-9.5Al-7.5W-X at. % alloys (X = 0-Temary, 0.05B, 0.01B, 0.05Zr, and 0.005B-0.05Zr at. %) are studied. Creep tests performed at 850 °C demonstrate that GB strength and cohesion limit the creep resistance and ductility of the ternary B- and Zr-free alloy due to intergranular fracture. Alloys with 0.05B and 0.005B-0.05Zr both exhibit improved creep strength due to enhanced GB cohesion, compared to the baseline ternary Co-9.5Al-7.5W alloy, but alloys containing 0.01B or 0.05Zr additions displayed no benefit. Atom-probe tomography is utilized to measure GB segregation, where B and Zr are demonstrated to segregate at GBs. A Gibbsian interfacial excess of 5.57 ± 1.04 atoms nm-2 was found for B at a GB in the 0.01B alloy and 2.88 ± 0.81 and 2.40 ± 0.84 atoms nm-2 for B and Zr, respectively, for the 0.005B-0.05Zr alloy. The GBs in the highest B-containing (0.05B) alloy exhibit micrometer-sized boride precipitates with adjacent precipitate denuded-zones (PDZs), whereas secondary precipitation at the GBs is not present in the other four alloys. The 0.05B alloy has the smallest room temperature yield strength, by 6 %, which is attributed to the PDZs, but it exhibits the largest increase in creep strength (with an ~2.5 order of magnitude decrease in the minimum strain rate for a given stress at 850 °C) over the baseline Co-9.5Al-7.5W alloy.