Combination of the magnetic dinuclear chromium(III) anion [Cr2(C2O4)(NCS)8]4 with the organic ET π-donor (ET = BEDT-TTF = bis(ethylenedithio)tetrathiafulvalene) yields two novel molecular hybrids (ET)n[Cr2(C2O4)(NCS)8] (1:n = 5; 2:n = 8). The particular arrangement of the organic units in the former leads to an unprecedented two-dimensional organic sublattice nearly similar to that observed in κ-phase structures. The packing of the ET units in 2 is near that observed in β-phase.