In the present work, we reported an excellent magneto-caloric effect (MCE) of a binary Gd63Ni37 amorphous alloy. The amorphous features of the Gd63Ni37 as-spun ribbons were ascertained by their X-ray diffraction pattern, differential scanning calorimetry (DSC) curve and their magneto-caloric behaviors. The Gd63Ni37 amorphous ribbon exhibits rather high magnetic entropy change peak (−ΔSmpeak), refrigeration capacity (RC) and adiabatic temperature rise (ΔTad). The binary Gd63Ni37 amorphous alloy is expected to play an important role in developing high performance multi-component Gd-Ni-based amorphous magnetic refrigerants.