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A novel type of exciton–phonon bound state—interlayer polaron—in a double‐layer 2D semiconductor with transition metal dichalcogenides as an example, is predicted. In these systems, the interaction of the interlayer exciton with the soft modes of out‐of‐plane lattice vibrations caused by van der Waals forces and flexural rigidity gives rise to a bound quasiparticle. The energy and effective mass of the formed polaron for weak and strong exciton–phonon coupling regimes are calculated and analyzed. Possible manifestations of these effects in transport‐ and spectroscopy‐related experiments are discussed.

Interlayer Exciton–Polaron in Atomically Thin Semiconductors