A method of forming a capacitor structure and manufacturing a semiconductor device, the method of forming a capacitor structure including sequentially forming a first mold layer, a supporting layer, a second mold layer, an anti-bowing layer, and a third mold layer on a substrate having a conductive region thereon; partially removing the third mold layer, the anti-bowing layer, the second mold layer, the supporting layer, and the first mold layer to form a first opening exposing the conductive region; forming a lower electrode on a sidewall and bottom of the first opening, the lower electrode being electrically connected to the conductive region; further removing the third mold layer, the anti-bowing layer, and the second mold layer; partially removing the supporting layer to form a supporting layer pattern; removing the first mold layer; and sequentially forming a dielectric layer and upper electrode on the lower electrode and the supporting layer pattern.