The optimized geometries, adiabatic electron affinities, vertical electron affinities, vertical electron detachment energies (for the anions), and IR-active vibrational frequencies have been predicted for the long linear carbon chains HC2n+1H (n = 4-11). The B3LYP density functional combined with DZP and TZ2P basis sets was used in this theoretical study. These methods have been extensively calibrated versus experiment for the prediction of electron affinities (Chem. Rev. 2002, 102, 231). The computed physical properties are discussed and compared with the even carbon chains HC2nH. The predicted electron affinities form a remarkably regular sequence: 2.12 eV (HC9H), 2.42 eV (HC11H), 2.66 eV (HC13H), 2.85 eV (HC15H), 3.01 eV (HC17H), 3.14 eV (HC19H), 3.25 eV (HC21H), and 3.35 eV (HC23H). These electron affinities are as much as 0.4 eV higher than those for analogous even carbon chains. The predicted structures display an intermediate cumulene-polyacetylene type of bonding, with the inner carbons appearing cumulenic and the outer carbons polyacetylenic.