Laves-phase compounds with the hexagonal C14-type structure Zr(Cr1-xFex)2 (x = 0.3-0.7) were charged to maximum H capacity, which ranged from 3.6 to 2.5 H/f.u. for increasing x. The biggest cell volume expansion was 22%. Magnetic properties were investigated with magnetometry and Mössbauer spectroscopy. The hydrides exhibited spin-glass behavior, similar to their parent compounds, but with larger Fe moments and lower freezing temperatures. Electric hyperfine interactions were measured in the 78-350 K temperature range at the Fe sites and at the Zr site, using 57Fe MS and 181Ta TDPAC, respectively. Activation energies for H jump diffusion were determined by these two complementary techniques, yielding 72(4) and 246(30) meV respectively. © 2002 Elsevier B.V. All rights reserved.