The use of recyclable forms of sulfur will exclude the risk of sediment reacidification and reduce the cost of bioleaching process. Three different forms of sulfur (namely sulfur powder, prills and pieces) were used to examine the utilization and recycle of sulfur, used as energy substrate for sulfur-oxidizing bacteria (SOB) in the bioleaching of heavy metal-contaminated sediments. The results showed that despite their relatively smaller surface areas, the efficiency of metal bioleaching with sulfur prills and pieces were comparable to that with sulfur powder. After 13 days of bioleaching, 71–74% of Zn, 58–62% of Cu, and 22–31% of Cr could be leached from the sediments, respectively. During bioleaching, most of the oxidizable and reducible forms of metals were transformed to acid soluble, posing a favorable condition for final metals removal. Sulfur recycling experiments showed that the recovered sulfur prills and pieces were as the same effective in pH reduction as fresh sulfur, revealing the feasibility of eventual reuse of the recycled sulfur in the bioleaching process. Further studies are required to testify the performance of these recyclable forms of sulfur in future large-scale bioleaching reactor.