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Performance of the group IV monochalcogenide GeSe in solar cells, electronic, and optoelectronic devices is expected to improve when high‐quality single crystalline material is used rather than polycrystalline films. Crystalline flakes represent an attractive alternative to bulk single crystals as their synthesis may be developed to be scalable, faster, and with higher overall yield. However, large – and especially large and thin – single crystal flakes are notoriously hard to synthesize. Here it is demonstrated that vapor‐liquid‐solid growth combined with direct lateral vapor‐solid incorporation produces high‐quality single crystalline GeSe ribbons with tens of micrometers size and controllable thickness. Electron microscopy shows that the ribbons exhibit perfect equilibrium (AB) van der Waals stacking order without extended defects across the entire thickness, in contrast to the conventional case of substrate‐supported flakes where material is added via layer‐by‐layer nucleation and growth on the basal plane. Electrical measurements show anisotropic transport and a high Hall mobility of 85 cm² V⁻¹ s⁻¹, on par with the best single crystals to date. Growth from mixed GeSe and SnSe vapors, finally, yields ribbons with unchanged structure and composition but with jagged edges, promising for applications that rely on ample chemically active edge sites, such as catalysis or photocatalysis.

The integration of dissimilar materials into heterostructures is a mainstay of modern materials science and technology. An alternative strategy of joining components with different electronic structure involves mixed‐dimensional heterostructures, that is, architectures consisting of elements with different dimensionality, for example, 1D nanowires and 2D plates. Combining the two approaches can result in hybrid architectures in which both the dimensionality and composition vary between the components, potentially offering even larger contrast between their electronic structures. To date, realizing such heteromaterials mixed‐dimensional heterostructures has required sequential multi‐step growth processes. Here, it is shown that differences in precursor incorporation rates between vapor–liquid–solid growth of 1D nanowires and direct vapor–solid growth of 2D plates attached to the wires can be harnessed to synthesize heteromaterials mixed‐dimensional heterostructures in a single‐step growth process. Exposure to mixed GeS and GeSe vapors produces GeS_1−xSe_xvan der Waals nanowires whose S:Se ratio is considerably larger than that of attached layered plates. Cathodoluminescence spectroscopy on single heterostructures confirms that the bandgap contrast between the components is determined by both composition and carrier confinement. These results demonstrate an avenue toward complex heteroarchitectures using single‐step synthesis processes.