The thermoelectric performance of XMg2Bi2 (X = Sr, Ba) materials is systematically investigated through integrated first-principles calculations, Boltzmann transport theory, and a two-channel model in this work. The temperature-activated static-dynamic transition in X (X = Sr, Ba) atoms vibrations induces a Janus effect of phonons, facilitating dual phonon transport regimes characterized by normal phonon and diffusons. The comparable ionicity between X2+ (X = Sr, Ba) and [Mg2Bi2]2- layers disrupts the conventional Zintl-phase characteristics, leading to an atypically isotropic lattice thermal conductivity within their materials. Concurrently, charge-insulating X2+ (X = Sr, Ba) layers restrict out-of-plane carrier mobility, creating a distinctive two-dimensional (2D) electronic transport framework superimposed on three-dimensional (3D) phonon dynamics. By disentanglement of the cross-dimensional transport phenomena through a two-channel model and multicarrier scattering analysis, the XMg2Bi2 (X = Sr, Ba) materials achieve remarkable thermoelectric performance with the optimal figure of merits (ZTmax) of 1.5 (p-type) and 1.9 (n-type) at 600 K, respectively.