In this work, two thiol-type reagents, thioglycolic acid (TGA) and mercaptopropionic acid (MPA), were firstly exploited and compared as aegirite depressants with sodium oleate (NaOl) as the collector to separate specularite from aegirite by flotation. The adsorption performances and mechanisms of TGA and MPA on aegirite surface were investigated via flotation experiments, Zeta potential tests, adsorption measurements, contact angle dimensions, and surface characterizations. The results of flotation indicated that TGA and MPA exhibited a considerable depression impact on the flotation of aegirite but little effect on specularite. TGA depicted more excellent depression performance than MPA, which was confirmed by HLB calculation. The results demonstrated that TGA and MPA favorably adsorbed on aegirite surface instead of specularite, hindering the subsequent adsorption of NaOl on specularite and resulting in the surface being hydrophilic. XPS results revealed that TGA and MPA were significantly adsorbed on the surface of aegirite through an interaction between the carboxyl and thiol groups of the depressants and the Si and Fe on the surface of aegirite.