The 1997 Formula 1 world champion had already been on the front row at the track named after his father three times, twice in F1 on his first two outings there with Williams, then last year in NASCAR's second-tier series.
However, pole had eluded him at the venue until this weekend. His best finish at the venue was second in his first Canadian Grand Prix in 1996. Last year he finished third in the Nationwide Series event, having led the race for a single lap.
This year Villeneuve is driving the #22 Penske Dodge that Sprint Cup regular Brad Keselowski has taken to victory lane twice this season, while Kurt Busch drove it to a dominant win from pole position last Saturday at Watkins Glen.
Villeneuve, who had been fastest in the final practice ahead of qualifying, has entered six NASCAR Nationwide Series events, all of them on road courses, most recently finishing third at Road America while making his first start for Penske Racing.
"If there's one place that you want to be quick, it's at home," said Villeneuve. "This is a special track as it bares my father's name. I've raced here 14 or 15 times, so there's a lot of history. It's good when you can get to a track and from the moment you get going, the car is great."
He added: "I did make my lap on the third lap, which isn't the way to go. That shows that our race pace should be good because our tyres are holding up. That gives us a lot of confidence for tomorrow."
Indianapolis 500 polesitter and Villeneuve's Penske team-mate Alex Tagliani secured an all-Canadian front row, while Braun Racing's Jason Leffler was third and best of the series regulars. Former F1 racer Scott Speed was fourth for Kevin Harvick's team, while Joe Gibbs Racing's Michael McDowell rounded out the top five in qualifying.
Robby Gordon was sixth fastest and best among the Sprint Cup regulars in the entry. Watkins Glen Cup winner Marcos Ambrose, Carl Edwards and Trevor Bayne were all on Cup duty at Michigan on Friday and will start from the back of the grid in Saturday's race.
The race is expected to be the final competitive outing of Patrick Carpentier's career and he will be starting from eighth place. He will be driving for Pastrana Waltrip Racing.