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Intrinsic 2D ferromagnetic semiconductors are an important class of materials for spin‐charge conversion applications. Cr 2 Ge 2 Te 6  retains long‐range magnetic order in the bilayer at cryogenic temperatures and shows complex magnetic interactions with considerable magnetic anisotropy. Here, a series of structural, magnetic, X‐ray scattering, electronic, thermal transport and first‐principles calculation studies are performed, which reveal that localized electronic charge carriers in Cr 2 Ge 2 Te 6  are dressed by the surrounding lattice and are involved in polaronic transport via hopping that is observed via magnetocrystalline anisotropy. This opens the possibility for manipulation of charge transport in Cr 2 Ge 2 Te 6 —based devices by electron–phonon‐ and spin–orbit coupling‐based tailoring of polaron properties.

Polaronic Conductivity in Cr 2 Ge 2 Te 6 Single Crystals