Intermetallic alloy ZrCo is a good material for storing tritium (T). However, ZrCo is prone to disproportionation reactions during the process of charging and discharging T. Alloying atoms are often added in ZrCo, occupying the Zr or Co site, in order to restrain disproportionation reactions. Meanwhile, T often decays into helium (He), and the purity of T seriously decreases once He escapes from ZrCo. Therefore, it is necessary to understand the influence of alloying atoms on the basic stability property of He. In this work, we perform systematical ab initio calculations to study the stability property of He in ZrCoH3 (ZrCo adsorbs the H isotope, forming ZrCoH3). The results suggest that the He atom will undergo displacements of 0.31 and 0.12 Å when it substitutes for Co and Zr, respectively. In contrast, the displacements are very large, at 0.67–1.09 Å, for He replacing H. Then, we introduce more than 20 alloying atoms in ZrCo to replace Co and Zr in order to examine the influence of alloying atoms on the stability of He at H sites. It is found that Ti, V, Cr, Mn, Fe, Zn, Nb, Mo, Tc, Ru, Ta, W, Re, and Os replacing Co can increase the substitution energy of H by the He closest to the alloying atom, whereas only Cr, Mn, Fe, Mo, Tc, Ru, Ta, W, Re, and Os replacing Co can increase the substitution energy of H by the He next closest to the alloying atom. The influence of the alloying atom substituting Zr site on the substitution energies is inconspicuous, and only Nb, Mo, Ru, Ta, and W increase the substitution energies of H by the He closest to the alloying atom. The increase in the substitution energy may suggest that these alloy atoms are conducive to fix the He atom in ZrCo and avoid the reduction in tritium purity.