Recent work on sputtered films of amorphous GdCo and GdFe alloys has shown that these films have large perpendicular anisotropy, which has been attributed principally to a pair‐ordering mechanism involving transition metal atoms. Chaudhari and Cronemeyer,1 however, have found Gd‐Co pairs to be dominant in sputtered Gd‐Co‐Mo films. We have observed that evaporated amorphous films in the Gd‐Fe binary system display strong perpendicular anisotropy over the composition range Gd8Fe92 to Gd33Fe67. In the evaporated Ge‐Co system, however, anisotropy is in‐plane when the Gd content exceeds 10%, with the direction of the easy axis of magnetization determined by the position of the Gd and Co evaporation sources. Assuming that the deposition processes are the same in both alloys, it seems likely that different pairs are dominant in the two alloy systems. We have established that Fe‐Fe is the dominant pair in GdFe alloys by fitting sublattice magnetizations from molecular field theory to the experimental anisotropy data.