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Tailorable magnetic properties and magneto-caloric effect were achieved in the Gd-Co binary amorphous alloys. It was found that the Curie temperature (Tc) of the GdxCo100-x (x=50, 53, 56, 58, 60) metallic glasses can be tuned by changing the concentration of Gd as Tc =708.8-8.83x, and the mechanism involved was investigated. On the other hand, a linear correlation between the peak value of magnetic entropy change (-Δ Smpeak) and Tc-2/3 is found in the amorphous alloys with a linear correlation coefficients of above 0.992. Therefore, the -ΔSmpeak of the Gd-Co binary amorphous alloys under different magnetic fields can be easily tailored by adjusting the composition of the alloy.