In the recent past, MnTe has proven to be a crucial component of the intrinsic magnetic topological insulator (IMTI) family

{[MnTe]}_{m} {[{Bi}_{2} {Te}_{3}]}_{n}

, which hosts a wide range of magnetotopological properties depending on the choice of

m

and

n

. However, bulk crystal growth allows only a few combinations of

m

and

n

for these IMTIs due to the strict limitations of the thermodynamic growth conditions. One way to overcome this challenge is to utilize the atomic layer-by-layer molecular beam epitaxy (MBE) technique, which allows arbitrary sequences of

{[MnTe]}_{m}

and

{[{Bi}_{2} {Te}_{3}]}_{n}

to be formed beyond the thermodynamic limit. For such MBE growth, finding optimal growth templates and conditions for the parent building block, MnTe, is a key requirement. Here, we report that two different hexagonal phases of MnTe–nickeline (NC) and zinc-blende/wurtzite (ZB-WZ) structures, with distinct in-plane lattice constants of

4.20 \pm 0.04

and

4.39 \pm 0.04 Å

, respectively–can be selectively grown on

c

-plane

{Al}_{2} O_{3}

substrates using different buffer layers and growth temperatures. Moreover, we provide comparative studies of different MnTe phases using atomic-resolution scanning transmission electron microscopy, and we show that ZB- and WZ-like stacking sequences can easily alternate between the two. Surprisingly,

{In}_{2} {Se}_{3}

buffer layer, despite its lattice constant (

4.02 Å

) being closer to that of the NC phase, fosters the ZB-WZ instead, whereas

{Bi}_{2} {Te}_{3}

, sharing the same lattice constant (

4.39 Å

) with the ZB-WZ phase, fosters the NC phase. These discoveries suggest that lattice matching is not always the most critical factor determining the preferred phase during epitaxial growth. Overall, this will deepen our understanding of epitaxial growth modes for chalcogenide materials and accelerate progress toward new IMTI phases as well as other magnetotopological applications.

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