The new magnetic refrigeration (MR) technology, which uses the magnetocaloric effect (MCE) of materials for refrigeration, has shown apparent advantages over the compression refrigeration of freon and other gases. Therefore, how to obtain materials with excellent magnetic entropy change near room temperature is of great significance for the realization of MR. In order to achieve high Tc of a Gd-based amorphous alloy, Gd45Co50Al5amorphous alloy with good room temperature MCE was selected, and a series of Gd45Co50−xFexAl5(x = 2, 5, 10) amorphous alloys were prepared by adding Fe instead of Co. In this paper, the effect of Fe addition on the Curie temperature, and the magnetic entropy change in the alloys, were studied thoroughly. The results show that the Curie temperature is increased to 281 K by adding 5% Fe elements, which is mainly related to the enhanced 3d-3dinteraction of transition elements caused by Fe addition, and the maximum value of magnetic entropy change is 3.24 J/(kg·K) under a field of 5 T. The results are expected to provide guidance for further improving the room temperature MCE of Gd-based amorphous alloys.