The longitudinal relaxation times of C-13 nuclei and NOE enhancement factors for 2-bromopyridine (1), 6-bromo-9-methylpurine (2), 3,5-dibromopyridine (3), 2,4-dibromopyrimidine (4), and 2,4,6-tribromopyrimidine (5) have been measured at 25 degrees C and B-0 = 11.7 T. The most important contributions to the overall relaxation rates of nonbrominated carbons, i.e., the relaxation rates due to the (CH)-C-13-H-1 dipolar interactions and the shielding anisotropy mechanism, have been separated out. For 3 and 5, additionally, the T-2,T-Q(N-14) values have been established from N-14 NMR line widths. All of these data have been used to determine rotational diffusion tensors for the investigated molecules. The measured saturation recovery curves of brominated carbons have been decomposed into two components to yield relaxation times, which after proper corrections provided parameters characterizing the scalar relaxation of the second kind for C-13 nuclei of Br-79- and Br-81-bonded carbons. These parameters and theoretically calculated quadrupole coupling constants for bromine nuclei have allowed the values of one-bond (CBr)-C-13-Br-79 spinspin coupling constants to be calculated. Independently, the coupling constants and magnetic shielding constants of the carbon nuclei have been calculated theoretically using the nonrelativistic and relativistic DFT methods F/6-311++G(2d,p)/PCM and so-ZORA/F/TZ2P/COSMO (F = BH and H or B3LYP), respectively. The agreement between the experimental and theoretical values of these parameters is remarkably dependent on the theoretical method used.