We present measurements of the first-and third-harmonic voltage response in ac electronic transport measurements, representing the linear (ohmic) and nonlinear resistivity, respectively, of the quasi-two-dimensional (2D) organic superconductors k-(BEDT-TTF) 2 X. Nonlinear transport is a sensitive tool to probe the microgeometry of the electronic system in high-quality single crystals. For the title compounds, the normalconducting metallic state in the vicinity of the Mott metal-insulator (MI) transition and critical endpoint is known to be highly unusual. Our results reveal large current-induced intrinsic inhomogeneities, at high current densities most pronounced at the so-called T Ã anomaly, which characterizes the anomalous metallic state. The observed nonlinearities in the interlayer transport do not depend on frequency and cannot be ascribed to a simple Joule heating mechanism in a resistor network. Furthermore, we find evidence supporting the notion of electronic phase separation induced by the Mott critical endpoint. The observed dependence of the generated thirdharmonic voltage on the current density reveals a systematic behavior suggesting that current-induced electronic inhomogeneities are more pronounced for more strongly correlated systems.ß 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim 1 Introduction In the last years, the quasi-twodimensional organic charge-transfer salts (BEDT-TTF) 2 X, where BEDT-TTF (bis-ethylenedithio-tetrathiafulvalene, commonly abbreviated as ET) represents C 6 S 8 [(CH 2 ) 2 ] 2 , have attracted considerable attention as model systems for studying the physics of correlated electrons and the Mott metal-insulator (MI) transition in reduced dimensions [1,2]. Recently, new routes of research also include the notion of quantum criticality and non-Fermi liquid behavior in these materials [3] as well as the simultaneous occurrence of ferroelectricity and magnetic ordering within the Mott insulating state [4]. In this paper, we address the unresolved question of the nature of the anomalous metallic state in the vicinity of the Mott transition, which -in general -can be radically different compared to the electronic band states in conventional metals. For example, close to a Mott MI transition, pseudogap behavior or an intrinsic electronic phase separation on the nanoscale is discusssed, e.g., in high-T c cuprates and organic superconductors k-(ET) 2 X with polymeric anions X À ¼ Cu[N(CN) 2 ]Z À (Z ¼ Br, Cl) or