Avoiding the formation of cracks to ensure a reliable printability and a good stability is crucial in the laser additive manufacturing of alloys. Contrary to previous studies that have generally tried to decrease the liquid film and solidification range, in this work, we innovatively utilized segregation engineering and abundant cell boundaries to introduce liquid backfilling as well as a network of segregation phases to alleviate thermal stress, consequently eliminating hot cracking. More specifically, zirconium was introduced into a nickel-based superalloy to form a continuous interdendritic liquid film during the laser additive manufacturing process. It was found that the continuous intermetallic Ni₁₁Zr₉ segregation phase decorated the cell boundaries, and cracks were completely eliminated in the as-printed Haynes 230 alloys when their Zr content reached 1 wt.%. Moreover, this continuous Ni₁₁Zr₉ network layer was able to act as a “skeleton” to significantly improve the yield strength of the as-printed samples. Following appropriate heat treatment, these Zr-modified Haynes 230 alloys exhibited an extraordinary combination of strength and plasticity, which were superior to those of the previously reported Haynes 230 alloy. These findings provide a new alloy design route for the laser additive manufacturing of crack-free alloys with excellent mechanical properties.