This study aimed to address the challenges encountered in traditional bulk wave delamination detection methods characterized by low detection efficiency. Additionally, the limitations of guided wave delamination detection methods were addressed, particularly those utilizing reflected waves, which are susceptible to edge reflections, thus complicating effective defect extraction. Leveraging the full waveform inversion algorithm, an innovative approach was established for detecting delamination defects in multi-layered structures using ultrasonic guided wave arrays. First, finite element modeling was employed to simulate guided wave data acquisition by a circular array within an aluminum-epoxy bilayer structure with embedded delamination defects. Subsequently, the full waveform inversion algorithm was applied to reconstruct both regular and irregular delamination defects. Analysis results indicated the efficacy of the proposed approach in accurately identifying delamination defects of varying shapes. Furthermore, an experimental platform for guided wave delamination defect detection was established, and experiments were conducted on a steel-cement bilayer structure containing an irregular delamination defect. The experimental results validated the exceptional imaging precision of our proposed technique for identifying delamination defects in multi-layered boards. In summary, the proposed method can accurately determine both the positions and sizes of defects with higher detection efficiency than traditional pulse-echo delamination detection methods.