ability to carry traveling waveguide modes at visible and near-infrared energies. [12] Van der Waals (vdWs) nanowires carrying axial screw dislocations are of particular interest for 3D twistronics. [13] Eshelby twist due to the screw dislocation [14] endows such wires with an inherent chiral structure in which the progressive rotation of the crystal axes translates (at the unit cell level) into interlayer twist that is stabilized by the dislocation and precisely (to ≈1/100°) [15] tunable via the nanowire diameter. The underlying twist moiré, realized here on a helicoid surface rather than a planar vdWs interface (IF) as in the conventional twisted homo-and heterostructures, [16] can modulate the bandgap and the local optoelectronic properties. [17] vdWs nanowires have been synthesized with high crystal quality using vapor-liquid-solid (VLS) growth, in which a liquid catalyst drop at the tip of the growing wire transports material from the vapor phase to the nanowire growth front. As in the growth of conventional 3D-crystalline (e.g., Si, Ge) nanowires, [18] the catalyst thus defines the positioning on the substrate and the diameter of the growing nanowire. In addition, in the growth of layered nanowires, the VLS catalyst defines the stacking of layers, which can be longitudinal, that is, with layer stacking along the wire axis, [15] or transverse, that is, ribbon-like with layers aligned along the wire axis. [3] Modifications of the catalyst have been shown to yield intermediate morphologies with tilted vdWs layering. [19] While posing significant synthesis challenges, ultrathin 3D-crystalline semiconductor nanowires have been realized for a variety of materials, including Si, [20,21] Ge, [22][23][24] ZnS, [25] CsPbBr 3 , [26] Bi 2 S 3 , [27] GaSb, [28] ZnSe, [29] InAs, [30] Ga 2 O 3 , [31] Mo 6 Te 6 , [32] etc., where they displayed size-dependent properties substantially different from their thicker counterparts such as different crystal orientations, [20,28] absence of defects such as stacking faults or twins, [30] strong quantum confinement, [21,26,33,34] large anisotropic lattice expansion, [25] intrinsic room temperature ferromagnetism, [25] unusually high thermal conductivity, [35] etc. In addition, dislocated, Eshelbytwisted 3D-crystalline nanowires (PbSe, PbS, [36] InP [37] ) show an enhanced twist rate at ultrathin diameters compared to Eshelby's continuum model, [14] attributed to surface relaxation effects. [37] In contrast to 3D-crystalline materials, ultrathin vdWs nanowires have remained elusive so far. Reaching the ultrathin regime is critical for addressing fundamental questions 1D nanowires of 2D layered crystals are emerging nanostructures synthesized by combining van der Waals (vdW) epitaxy and vapor-liquid-solid (VLS) growth. Nanowires of the group IV monochalcogenide germanium sulfide (GeS) are of particular interest for twistronics due to axial screw dislocations giving rise to Eshelby twist and precision interlayer twist at helical vdW interfaces. Ultrathin vdW nanowires have not been rea...