High-resolution 95.2 MHz deuteron NMR spectra were obtained from dilute ether solutions of the monodeuteromethyl halides (X = Cl, Br, I). Small quadrupole splittings were resolved, resulting from molecular alignment by the 14.57 T field. These splittings relate the deuterium quadrupole coupling constants (qcc) to the anisotropy in the molecular diamagnetic susceptibility (Δξ). The results are consistent with literature qcc and Δξ values for CH3CI and CH3 Br, but suggest that Δξ of CH3I determined by microwave spectroscopy is high by about 14%. A survey of literature qcc data for the complete series of halomethanes is given. The data indicate a good agreement between qcc's found from gas-phase studies (microwave), low-temperature solid-state NMR and NQR experiments, and investigations using certain well-chosen liquid crystal mixtures. The values judged to be most accurate were combined with quadrupole splitting data to obtain molecular and bond susceptibilities for this series of compounds.