 This paper presents a new technique for creating helically decorated microcylinders, which can be used to create microspheres with helically patterned compartments. This technique involves twisting microfibers while they are being ejected through a nozzle, resulting in helically decorated microcylinders. These cylinders can then be used to form microspheres by interfacial shape-shifting. This article was authored by Manje Gil, Siangjin Moon, J1 Yoon, and others.