Various reaction mechanisms for the reaction between N2OH+ and CH4 have been explored theoretically at the MP2 6-31G** level. Also computed were the structure and thermodynamic state functions for several neutral molecules, notably N2O, CH4 and C2H6 and ions (CH5+, C2H5+, C2H7+, N2OH+). These results were combined with a Fourier transform ion cyclotron resonance study of the reactions of N2OH+ with CH4 or C2H6. Both studies suggest that the title hydride transfer, while thermodynamically favorable, is not Kinetically preferred under thermal conditions in the gas phase. © 1995.