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Squeezing bubbles and impurities out of interlayer spaces by applying force through a few-layer graphene capping layer leads to van der Waals heterostructures with the ultraflat structure free from random electrostatic potential arising from charged impurities. Without the graphene capping layer, a squeezing process with an AFM tip induces applied-force-dependent charges of Δn ∼ 2 × 1012 cm-2 μN-1, resulting in the significant intensity of trions in photoluminescence spectra of MoSe2 at low temperature. We found that a hBN/MoSe2/hBN prepa