Adiabatic connection models (ACMs), which interpolate between the limits of weak and strong interaction, are powerful tools to build accurate exchange–correlation functionals. If the exact weak-interaction expansion from the second-order perturbation theory is included, a self-consistent implementation of these functionals is challenging and still absent in the literature. In this work, we fill this gap by presenting a fully self-consistent-field (SCF) implementation of some popular ACM functionals. While using second-order perturbation theory at weak interactions, we have also introduced new generalized gradient approximations (GGAs), beyond the usual point-charge-plus-continuum model, for the first two leading terms at strong interactions, which are crucial to ensure robustness and reliability. We then assess the SCF–ACM functionals for molecular systems and for prototypical strong-correlation problems. We find …