Gd54Fe36B10−xSix(x= 0, 2, 5, 8, 10) amorphous ribbons were fabricated by melt-spinning technique. Based on the molecular field theory, the magnetic exchange interaction was analyzed by constructing the two-sublattice model and deriving the exchange constantsJGdGd,JGdFeandJFeFe. It was revealed that appropriate substitution content of Si for B can improve the thermal stability, maximum magnetic entropy change and widened table-like magnetocaloric effect of the alloys, while excessive Si will lead to the split of the crystallization exothermal peak, inflection-like magnetic transition and deterioration of magnetocaloric properties. These phenomena are probably correlated to the stronger atomic interaction of Fe-Si than that of Fe-B, which induced the compositional fluctuation or localized heterogeneity and then caused the different way of electron transfer and nonlinear variation in magnetic exchange constants, magnetic transition behavior and magnetocaloric performance. This work analyzes the effect of exchange interaction on magnetocaloric properties of Gd-TM amorphous alloys in detail.