The controllable preparation of materials with unique structures and morphologies has become an important field in the development of nanomaterials. In this study, Sb2S3 was used as the evaporation source to controllably prepare Sb2S3 crystals with various morphologies under a vacuum. At 873 K and 30 min, antimony sulfide in the form of cauliflower-like was effectively made. At the same temperature and for 60 min, tubular antimony sulfide was formed. The initial forming conditions of fascicle-like antimony sulfide were at 873 K and 100 min and did not change with the increase in temperature. During the evaporation process, some antimony sulfide will condense into lumps, showing irregular feather-like and round particles. The products prepared by this method were analyzed and tested. The results showed that the grade of antimony sulfide prepared by this method was further improved, and the content of Sb and S increases by 1.64% and 1.21% on average. This method offers a simple production process, a more regular product shape, and does not require the use of any additives.