<p>Fe-based bulk metallic glasses (BMGs) with high B and Gd content have potential applications as coating materials for spent nuclear fuel shelf to ensure their safe long-term storage. The requirements for such materials are excellent glass-forming ability (GFA), mechanical properties and corrosion resistance, as well as high neutron absorption characteristics. Both B and Gd has the largest neutron or thermal neutron capture cross section among neutron absorbing elements. In this work, the alloys of Fe_70-<i>x</i>Cr_<i>x</i>Nb₄B₂₂Gd₄ (<i>x</i> = 0–10&#xa0;at.%) with high B and Gd content were designed, and the GFA, thermal stability and mechanical properties of which were investigated. The critical diameter of the glassy alloy rods is 3&#xa0;mm at Cr contents of 0, 2 and 4&#xa0;at.%, respectively, with the supercooled liquid temperature region (Δ<i>T</i>_x) greater than 45&#xa0;K. The fracture strength of alloy with Cr content of 2&#xa0;at.% is 3468&#xa0;MPa. The suitable GFA and excellent mechanical properties make Fe₆₈Cr₂Nb₄B₂₂Gd₄ BMG with high B and Gd contents as an ideal neutron absorption coating material with the potential for use in spent fuel storage shelf.</p>