The Mott insulator κ-(BEDT-TTF)2Cu[N(CN)2]Cl consists of molecular dimers arranged on an anisotropic triangular lattice. At low temperatures a pronounced dielectric anomaly is observed, and eventually a canted antiferromagnetic ground state forms. Optical spectroscopy clearly rules out charge imbalance and the existence of quantum electric dipoles with a dipolar-spin coupling. Here we suggest a novel form of spin-charge coupling where the prominent in-plane dielectric response in κ-(BEDT-TTF)2Cu[N(CN)2]Cl is explained by short-range discommensurations of the antiferromagnetic phase in the temperature range 30 K < T < 50 K, and by relaxation of charged domain walls in the ferromagnetic structure at lower temperatures.