The present invention provides a process for preparing ball-type desulfurizer with high sulfur capacity, comprising the following steps: placing initial balls in a rolling equipment; wetting the surface of the initial balls with an aqueous solution of an organic binder; then alternately adding non-crystalline iron oxide hydroxide and the aqueous solution of the organic binder to gradually form small balls of non-crystalline iron oxide hydroxide with high sulfur capacity and different diameters; and adjusting the shape of the small balls and then roasting or naturally drying the small balls. In the desulfurizer prepared by this method, the initial balls constitutes 0.98 wt %-9.03 wt % of the desulfurizer, the non-crystalline iron oxide hydroxide constitutes 90.29 wt %-98.62 wt % of the desulfurizer, and the organic binder constitutes 0.58 wt %-0.89 wt % of the desulfurizer. The present invention solves the problems that the desulfurizer with high sulfur capacity in the prior art has a high binder content and poor water resistance and diffusion performance, and provides a process for preparing a desulfurizer with high sulfur capacity, wherein a desulfurizer with high sulfur capacity and low binder content, good water resistance, good diffusion performance can be prepared.