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Thick hydride vapor phase heteroepitaxy of some III–V, II–VI, and III–VI binary and ternary semiconductor materials such as GaAs, GaP, GaP, GaAsxP1‐x, ZnSe, and GaSe is performed on GaAs substrates and orientation‐patterned GaAs templates. Up to 500 μm thick GaAs, GaP, GaP, GaAsxP1‐x, and ZnSe layers are deposited in single growths or after a regrowth. The GaSe layers deposited through van der Waals heteroepitaxy are up to 4–5 μm thick. When possible, growths are also performed homoepitaxially as the comparison of growth rate and layer quality indicates similar or better results in some of the heteroepitaxial cases. Material analysis using optical microscopy, scanning electron microscopy, atomic force microscopy, high‐resolution X‐ray diffraction, and energy dispersive X‐ray spectroscopy indicate smooth surface morphology, uniform layer thicknesses, high crystalline quality, and gradual substrate‐to‐layer material transition in the cases of heteroepitaxy. Respectively, the growths on the templates prepared by an optimized polarity inversion technique (assisted by molecular‐beam epitaxy) reveal excellent domain fidelity and good infrared transparency. The samples grown on templates are intended for frequency conversion devices operating in mid and longwave infrared. The layers grown on plain substrates are meant to support applications in optoelectronics, renewable energy, sensing, and solar cells.

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