Ab initio one-, two-, and three-bond C−C, C−N, and N−N spin−spin coupling constants, and one-bond C−H and N−H coupling constants have been computed using two different theoretical methods, SOPPA/(qzp,qz2p) and EOM-CCSD/(qzp,qz2p). Both EOM-CCSD (equation-of-motion coupled cluster singles and doubles) and SOPPA (second-order polarization propagator approximation) coupling constants correlate linearly with experimental data. In the great majority of cases, the computed EOM-CCSD C−C, C−N, N−N, and N−H coupling constants are in better agreement with experimental data than SOPPA values, although both levels of theory provide reasonable estimates of these couplings. EOM-CCSD consistently underestimates one-bond C−H coupling constants by about 10 Hz, and SOPPA values of 1J(C−H) are in better agreement with experimental data. The performance of SOPPA supports its use in future studies of coupling constants involving C, N, and H in larger chemical and biological systems.