Simpson, who is in his second year with the Vikings, was arrested by the Minnesota State Patrol and booked at 5:39 on Saturday morning, according to the Hennepin County Sherriff's jail roster.
According to a Minnesota State Patrol arrest report, a state trooper responded to a report of a stalled vehicle on Interstate-394 leaving Minneapolis.
Simpson, who had blurry eyes and slurred speech, said he was coming from the Pour House in downtown Minneapolis, but denied having been drinking. He failed a field sobriety test, was arrested and transported to the jail, where he refused a breath test.
He posted bail of $12,000 on Saturday afternoon, though formal charges from prosecutors are still pending.
Simpson was suspended for the first three games of the 2012 after pleading guilty to a drug-related charge in March 2012.
The Vikings signed Simpson shortly after the NFL suspended him, and his DWI occurred during the first year of the three-year probation sentence ordered by a Kentucky judge.
It remains to be seen how the arrest will affect Simpson's probation, or if he will face additional discipline from the league.
The Vikings said in a statement on Saturday morning that they "are aware of the matter involving Jerome Simpson. We are continuing to gather information and will have further comment at the appropriate time."
Simpson, who was plagued by a back injury after returning from his suspension in 2012, had been in the middle of a rebound season with the Vikings. He had caught 33 passes for a team-high 491 yards in nine games after re-signing with the team on a one-year deal in March.
This spring, Simpson talked about having a big year and earning a long-term deal with the Vikings.