Metal sorbent compositions for removing a metal contaminant from a fluid, such as removal of mercury from a coal-fired flue gas stream, and methods for making and using the same are provided. The subject metal sorbent compositions comprise an effective amount of an aqueous dispersion of microfine elemental sulfur particles on an adsorbent substrate, and optionally, a metal capture enhancing agent such as a halogen source and/or an oxidizing agent in an amount providing a metal capture enhancing effect on the metal sorbent composition. The subject metal sorbent compositions are prepared by drying an aqueous dispersion of microfine elemental sulfur particles on an adsorbent substrate, such as on a substrate of microfine particles of a refractory material and the like. Also provided are kits for use in preparing the subject compositions, and compositions produced by the methods. The subject compositions, kits and systems find use in a variety of different applications.