A single-crystal ³⁵Cl Zeeman NQR study of methylene chloride and its deuterated analog yielded a value of 0.068 for the asymmetry parameter. The directions between the field gradient Z axes correspond well with the interbond axes determined by X-ray crystallography and by microwave spectroscopy. For deuterochloroform the two resonances at 38.2441 and 38.3012 MHz have asymmetry parameters of 0.040 and 0.057, respectively, and the angle between the field gradient Z axes corresponds likewise to the Cl-C-Cl angles.