After a flawless showing to go fastest in the morning at the Circuit Gilles Villeneuve, the 20-year-old Red Bull driver followed up with a similar run in the afternoon.
It was the first time he had topped the times in any practice sessions this year.
"Yeah, that was a pretty good day for me, but I think Mercedes looked very fast in the longer runs," he said in a brief post-session comment.
Twenty-four hours after his impetuous performance at a pre-race news briefing, in which he threatened to "head-butt" his inquisitors, it was a perfect answer to those who had questioned his temperament after a series of incidents this season.
Verstappen clocked a best lap in one minute, 12.198 seconds to outpace nearest rival Kimi Raikkonen, the 2007 champion, of Ferrari by 0.130 seconds in the second session.
That left his Red Bull team-mate Daniel Ricciardo, who won the Monaco Grand Prix two weeks ago, down in third, four-tenths of a second adrift, ahead of championship leader and defending four-time champion Lewis Hamilton of Mercedes.
Sebastian Vettel, who trails Hamilton by 14 points in the title standings after six races, was fifth for Ferrari, seven-tenths off the pace ahead of Finn Valtteri Bottas in the second Mercedes.
The session, like the morning one, delivered two major incidents when Spaniard Carlos Sainz smacked the wall in his Renault, bringing a red-flag interruption for seven minutes, and later when Belgian Stoffel Vandoorne went into the barriers at Turn Eight, breaking the suspension of his McLaren.
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