The invention provides a preparation method of polycrystalline zinc selenide. The preparation method comprises the following steps that the surface of a polycrystalline zinc selenide sheet with the thickness of 30-50mm is treated to obtain a zinc selenide polished wafer with the roughness being less than Ra20, the zinc selenide polished wafer is cleaned with plasma, and the cleaned zinc selenide polished wafer is put on a graphite substrate; step 2, the zinc material is installed in a crucible; step 3, a graphite substrate depositor is mounted on a graphite crucible and then put in a chemical vapor deposition vacuum furnace; step 4, argon is introduced into the chemical vapor deposition vacuum furnace at room temperature; step 5, the crucible is heated, and the graphite substrate depositor is heated; step 6, the zinc starts to evaporate, hydrogen selenide gas carried by the argon is introduced into the graphite substrate depositor, and argon is introduced into the crucible; and step 7, after zinc evaporation is finished, introducing of the hydrogen selenide gas is stopped, the crucible is cooled, the graphite substrate depositor is cooled, and the final polycrystalline zinc selenide with the overall thickness of 60-100mm is obtained after being discharged from the furnace. According to the invention, the thick polycrystalline zinc selenide material can be prepared.