Methods of forming a polycrystalline compact for use in an earth-boring tool include sintering a plurality of hard particles with catalyst material to form a polycrystalline material that includes a plurality of inter-bonded particles of hard material integrally formed with the catalyst material and introducing at least a portion of the polycrystalline material to a reactive material to remove at least a portion of the catalyst material contained within the polycrystalline material. The reactive material may include at least one of a molten glass, an ionic compound, a leaching liquor, and a chemical plasma. The reactive material may be introduced to the polycrystalline material at a temperature of greater than or equal to a melting point thereof.