The invention relates to a method for synthesizing aminoacetonitrile and N,N-dimethylcyanamide by using methane and ammonia gas as raw materials, which is characterized by comprising the following steps: performing non-equilibrium plasma activation on methane and ammonia gas to generate carbon-containing and nitrogen-containing free radical active species, and performing one-step spontaneous reaction on the species to generate the target products. The method belongs to a one-step direct synthesis process, has the advantages of simplicity and cheap raw materials, does not use solvent and causes no pollution. Besides, the method is also applicable to synthesis of organic compounds from various C1-5 alkane, olefin and alkyne and ammonia gas. Moreover, in addition to the aminoacetonitrile and N,N-dimethylcyanamide, acetonitrile, ethylenediamine, 4,5-dihydro-5-methylpyrazole, aminopyrazole and other products can be also obtained through the plasma synthesis method.