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Flexible piezoelectric energy harvesters (f‐PEHs) have exhibited significant potential as long‐lasting self‐powered sources or sensor devices, as they can generate reliable and repeatable electricity under harsh and tiny mechanical bending cycles without restraints anywhere and anytime. Herein, a new approach for transferring piezoelectric ceramic thin films onto a single flexible substrate via piecemeal elimination of the sacrificial mica substrates is proposed. The crystallized piezoelectric BaTiO3thin film on a rigid mica substrate with electrodes and passivation layers is peeled off by means of a physical delamination process using sticky tape as the remover. The film is then transferred onto a flexible polyimide substrate using a polymer elastomer as a support. The fabricated BaTiO3thin‐film f‐PEH successfully converts an open‐circuit voltage of ≈0.5 V and a short‐circuit current of ≈30 nA from repeated mechanical bending deformations. The energy generation mechanism and performance of the perovskite BaTiO3thin‐film f‐PEH is supported using finite‐element analysis (FEA) with multiphysics simulations. The novel transfer techniques adopting the removal of sacrificial mica layers opens the door to various high‐performance flexible and wearable applications based on all‐inorganic materials. A piezoelectric BaTiO3thin film–based flexible energy harvester is fabricated by exfoliating the mica substrate. The well‐crystallized BaTiO3thin film on mica substrate is peeled off by a physical delamination process with sticky tape and then moved onto a flexible substrate. The fabricated flexible piezoelectric energy harvester generates an output performance of ≈0.5 V and ≈30 nA from mechanical bendings.