The chromadicarbaboranes CpCrC2Bn-3Hn-1 (8 <= n <= 12) are of interest in providing stable paramagnetic deltahedral metallaboranes among which the 12-vertex CpCrC2B9H11 has been synthesized by Hawthorne and co-workers. Density functional theory shows that the lowest-energy such structures, are quartet spin-state Cr(III) structures in which the central CrC2Bn_(3) units exhibit most spherical closo deltahedral geometries similar to those found in the borane dianions B(n)Hn(2-). Higher-energy doublet CpCrC2Bn-3Hn-1 (8 <= n <= 11) structures are found exhibiting central CrC2Bn_(3) isocloso deltahedral geometries, thereby providing a degree 6 vertex for the chromium atom. The lowest-energy CpCrC2Bn_H-3(n)_1 (8 <= n <= 11) structures all have both carbon atoms at degree 4 vertices. However, the lowest-energy CpCrC2B9H11 structures all have central CrC2B9 icosahedra and thus lack degree 4 vertices for the carbon atoms. For all of the CpCrC2Bn-3Hn-1 (8 <= n <= 12) systems the lowest-energy isomers are those with the maximum number of Cr-C edges in contrast to the related CpCoC2Bn-3Hn-1 systems.