Daniel Ray Hawkins, 33, and Benjamin Blake Lumpkin, 35, were arrested last week at a home on Flaherty Avenue in Wake Forest.
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The sheriff's office said the house was used to produce the hallucinogenic drug, Dimethyltryptamine or DMT.
The men were allegedly putting the drugs in vape pens.
A shotgun was also seized from the home.
According to the sheriff's office, there have only been three DMT labs located in North Carolina.
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Members of the Wake County Drugs and Vice Unit have found two of the three in the state's history.
The total street value of the bust was estimated to be almost $4 million.
Lumpkin and Hawkins were charged with Manufacture of a Schedule I, Maintaining a Dwelling, Possession of Precursors and Possession of Firearm by a Convicted Felon. Hawkins is currently in the Wake County Justice Center under an $835,000 bond and Lumpkin is there also under a $135,000 bond.