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Self-assembly of vertically aligned III–V semiconductor nanowires (NWs) on two-dimensional (2D) van der Waals (vdW) nanomaterials allows for integration of novel mixed-dimensional nanosystems with unique properties for optoelectronic and nanoelectronic device applications. Here, selective-area vdW epitaxy (SA-vdWE) of InAs NWs on isolated 2D molybdenum disulfide (MoS 2 ) domains is reported for the first time. The MOCVD growth parameter space ( i.e. , V/III ratio, growth temperature, and total molar flow rates of metalorganic and hydride precursors) is explored to achieve pattern-free positioning of single NWs on isolated multi-layer MoS 2 micro-plates with one-to-one NW-to-MoS 2 domain placement. The introduction of a pre-growth poly- l -lysine surface treatment is highlighted as a necessary step for mitigation of InAs nucleation along the edges of triangular MoS 2 domains and for NW growth along the interior region of 2D micro-plates. Analysis of NW crystal structures formed under the optimal SA-vdWE condition revealed a disordered combination of wurtzite and zinc-blend phases. A transformation of the NW sidewall faceting structure is observed, resulting from simultaneous radial overgrowth during axial NW synthesis. A common lattice arrangement between axially-grown InAs NW core segments and MoS 2 domains is described as the epitaxial basis for vertical NW growth. A model is proposed for a common InAs/MoS 2 sub-lattice structure, consisting of three multiples of the cubic InAs unit cell along the [21̄1̄] direction, commensurately aligned with a 14-fold multiple of the Mo–Mo (or S–S) spacing along the [101̄0] direction of MoS 2 hexagonal lattice. The SA-vdWE growth mode described here enables controlled hybrid integration of mixed-dimensional III–V-on-2D heterostructures as novel nanosystems for applications in optoelectronics, nanoelectronics, and quantum enabling technologies.