An elegant way for the controlled production of either cellulose fibers or hollow half spheres from trimethylsilyl cellulose (TMSC) via needleless electrospinning is reported. For this purpose trimethylsilyl celluloses (DS: 2.6-2.7) have been synthesized from three different cellulose sources, namely spruce pulp, AVICEL, and a viscose pulp. While TMSC from AVICEL is hardly processable via electrospinning, the use of viscose pulps leads to hollow semi spheres, whereas the spruce pulp based TMSC yields fibrous networks. The approach takes advantage of different degrees of molecular entanglements caused by differences in origin and molecular weight of the cellulosic material. These investigations may pave the way for further use of electrospun materials made from TMSC in, e.g., sensor devices.