Zinc sulfide (ZnS), which belongs to transition metal monochalcogenides, is a semiconductor material with wide direct band gap. It can potentially show some special applications (such as luminescence, phosphor, sensors, infrared window materials, photocatalysis) by changing the morphology, size, and crystal structure of semiconductor materials. However, ZnS nanospheres have not been studied as optical modulators until now. Herein, ZnS nanospheres are synthesized by the hydrothermal method and are used to realize optical modulators in an Er‐doped fiber laser. The evanescent field effect is utilized to incorporate the ZnS nanospheres on a tapered fiber. Furthermore, with the increase in pump power, the modulation interval gradually decreases to a minimum of 34.36 ns corresponding to the modulation frequency of 29.1 MHz, which is the highest modulation frequency to our knowledge in a ring cavity all‐fiber laser. These results demonstrate ZnS nanospheres together with the interaction of dispersion and nonlinearity in optical fibers can modulate the proposed lasers. This not only provides a new method for controlling the power and frequency of all optical modulators, but also marks an important step for ZnS materials in optics research and device applications.