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<i>Ophiocordyceps sinensis</i> has been utilized in China and adjacent countries for thousands of years as a rare functional food to promote health and treat diverse chronic diseases. In recent years, adulterants are usually identified in the processed products of wild <i>O. sinensis</i>. However, the effective adulteration examination has to be additionally performed except their routine test, and accordingly is time- and money-consuming. Recently, arsenic determination has become a necessary test for confirming whether the concentrations of inorganic arsenic are over the <i>O. sinensis</i> limit. In this work, the contents of total arsenic and As species in cultivated <i>O. sinensis, Cordyceps militaris</i>, and other edible fungi were determined by ICP-MS and HPLC-ICP-MS. The results suggest that the As speciation exhibits a species-specific behavior, and accompanies the effect of the As background. The proportions of unknown organic As and contents of total As may be considered as sensitive markers for discriminating wild <i>O. sinensis</i>. This result provides a novel clue for discriminating wild and artificially cultivated mushrooms/their products, with emphasis on arsenic markers for authenticating wild <i>O. sinensis</i>.