Hexagonal (C14) Laves-phase Zr(FexCr1-x)2 alloys with x = 0.3, 0.4, 0.5, 0.6 and 0.7 have been prepared by arc melting and the corresponding hydrides have been formed by hydrogen uptake at 1 atm pressure. X-ray diffractograms have been measured and analyzed with the Rietveld method. 57Fe Mossbauer spectra, measured at room temperature, could be fitted with two doubles with 3:1 area ratio, corresponding to the two Fe sites in the C14 structure. The quadrupole splitting (Δ) and isomer shift (δ) dependences on x are discussed in terms of volume and charge effects. The hydrides showed volume expansions of up to 22% without any crystal structure change. Both Mossbauer hyperfine parameters Δ and δ increased markedly in the hydrides as compared to the alloys. Tetrahedral hole radii have been calculated from measured crystalline parameters and their relationship to hydrogen site preferences is discussed.