The giant magnetoresistance effect DELTAR/R in magnetron-sputter deposited Fe/Cr multilayers is shown to depend strongly on deposition temperature. The largest values of DELTAR and magnetoresistance are found in structures deposited at congruent-to 125-degrees-C. Structures deposited at lower (congruent-to 30-degrees-C) or higher (congruent-to 200-degrees-C) temperatures exhibit lower DELTAR and DELTAR/R values. Low angle x-ray reflectivity and rocking curve data show that all the structures have well defined layers. However the largest giant MR values are found in structures which have the lowest high field resistivities, R, the longest structural coherence lengths and the narrowest (110) rocking curve widths. These results suggest that more perfect structures have intrinsically higher giant magnetoresistance.