The paper investigated the electrode delaminationbuckling of the layered system containing a through-the-width delaminationbetween the metallic electrode and the half-space piezoelectric substratebased on the finite deformation theory of elasticity and the biasing fieldtheory of the electroelastic body. The layered system in the plane strainproblem is subjected to the compressive strain-load parallel to the freesurface. Meanwhile, the theoretical model is reduced to the second kindCauchy-type singular integral equations by means of the Fourier integraltransform, the boundary conditions and the interfacial continuousconditions. The singular integral equations are solved numerically byutilizing Gauss-Chebyshev integral formulae. As an example, the layeredsystem of the metallic electrode Pt and piezoelectric substrate PZT-4 isconsidered. Numerical results for the critical strains of buckling and thecorresponding delamination buckling shapes are presented for, respectively,various ratios of the delamination length to thickness and the effect ofelectromechanical coupling in the piezoelectric substrate. The curves of thesingular oscillating factors in the delamination tip with respect to theratios of delamination length to thickness are also given.