Continuing studies based on measurements of the nuclear spin relaxation rates running via the SC2 mechanism (scalar relaxation of the second kind), we present in this work the results obtained for three bromo compounds: CBrCl3, (CH3)(3)CBr, and CBr4. A careful separation of saturation-recovery curves, measured for signals of C-17 nuclei at 7.05 and 11.7 T on two components, has provided the longitudinal SC2 relaxation rates of carbon signals in Br-79 and Br-81 containing isotopomers of the investigated compounds. These data have enabled experimental determination of spin-spin coupling constants and relaxation rates of quadrupole bromine nuclei, both types of parameters being hardly accessible by direct measurements. Investigation of the relaxation behavior of these molecules, being of similar size and shape, has provided quite different practical and interpretational problems which are likely to be encountered in relaxation studies of many other carbon-bromine systems. In order to evaluate the quality of the obtained experimental results, advanced theoretical calculations of the indirect (1)J(C-13,Br-79) coupling constants, magnetic shielding of carbon nuclei, and quadrupole coupling constants of bromines in the investigated compounds have been performed and compared with the experimental values. Relatively small divergences between experiment and theory have been found. The contributions of the relativistic effects to the values of the discussed parameters have been tentatively estimated.