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Abstract Specific ions can be intercalated into functional materials using the electrolyte gating technique, which has been widely used to regulate channel conductance in transistors and develop low‐power neuromorphic devices. However, in these devices, fundamental exploration of ion intercalation‐induced structural phase transitions remains largely overlooked and rarely explored. Here, the lithium‐based electrolyte gating technique is used to probe the collective interactions between ions, lattices, and electrons in a van der Waals ferroelectric semiconductor α‐In₂Se₃. Using a polymer electrolyte as the lithium‐ion reservoir and α‐In₂Se₃as the channel material, the intercalated lithium concentration via a gate electric field is modulated. This manipulation drives a phase transition in α‐In₂Se₃from a ferroelectric semiconductor to a dirty metal and finally to a metal, accompanied by a structural transformation. Concurrently, with enhanced intercalation, the ferroelectric hysteresis window progressively narrows and eventually disappears, indicating the evolution from switchable to non‐switchable polarization. This study represents a promising platform for the artificial construction of correlated material systems, enabling a systematic investigation into the interaction of ferroelectricity and electronic conduction using ion intercalation.