Seven carbon chain radicals NC_nS where n = 1-7 have been detected in a supersonic molecular beam by Fourier transform microwave spectroscopy. Although NCCS is found to have a bent structure and an asymmetric top spectrum, the five longer chains have linear heavy-atom backbones, and like the isovalent HC_nS chains, the electronic ground states of each alternate with even and odd numbers of carbon atoms: NC₄S and NC₆S have ²Π_1/2 ground states, while NC₃S, NC₅S, and NC₇S have ²Π_3/2 ground states. In addition, the lowest-rotational transitions of the NCS radical have been detected in both fine-structure levels in the same supersonic molecular beam source, allowing a precise determination of the ground state hyperfine coupling constants. The centimeter-wave spectra of NC₃S and the four longer chains have been fully characterized, and spectroscopic constants, including those that describe the lambda-type doubling and hyperfine structure from the nitrogen nucleus, have been determined to high precision. A complete account of the centimeter-wave spectrum of NCCS will be given by Nakajima et al. Predicted properties from UQCISD/cc-pVDZ ab initio calculations are also reported for the NC_nS chains up to NC₇S. All six new chains are highly polar and all are plausible candidates for astronomical detection because C_nS chains up to C₃S and C_nN chains up to C₅N are detected in both interstellar and circumstellar sources.