Gd2O3 nanoparticles surface‐modified with IPDI were compounded with epoxy. IPDI provided an anchor into the porous Gd2O3 surface and a bridge into the matrix, thus creating strong bonds between matrix and Gd2O3. 1.7 vol.‐% Gd2O3 increased the Young's modulus of epoxy by 16–19%; the surface‐modified Gd2O3 nanoparticles improved the critical strain energy release rate by 64.3% as compared to 26.4% produced by the unmodified nanoparticles. The X‐ray shielding efficiency of neat epoxy was enhanced by 300–360%, independent of the interface modification. Interface debonding consumes energy and leads to crack pinning and matrix shear banding; most fracture energy is consumed by matrix shear banding as shown by the large number of ridges on the fracture surface.
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