Matrix isolation and cryogenic thin film approaches have been employed for the synthesis, isolation, and characterization of 1:1 and 1:2 complexes of (CH3)(2)Zn with CH3OH and CH3SH. These complexes were characterized by a shifting of certain sensitive vibrational modes of the acid and base subunits in the complex. The ratio of the 1:1 and 1:2 complexes could be altered by changing the relative amounts of the two reagents employed in a given experiment or by warming the cryogenic thin film from 14 K to as high as 200 K. Merged jet mixtures of (CH3)(2)Zn with either CH3OH and its isotopomers or CH3SH were also pyrolyzed at temperatures as high as 370 degrees C. For the (CH3)(2)Zn/CH3OH pair, significant production of CH4 and CH2O was observed with minor amounts of C2H4. In the (CH3)(2)Zn/CH3SH experiments a substantial yield of(CH3)(2)S and CH4 was obtained. These pyrolytic reactions and products have not been reported previously and may have implications for the chemical vapor deposition of ZnO and ZnS.