After Paire had breezed to victory in less than two hours, French Number 1 Pouille, back where he won the winning point for his country in last year's final, battled from a set down to beat Roberto Bautista Agut in a classic five-setter 3-6 7-6(5) 6-4 2-6 6-4 in three hours 41 minutes.
France's inspirational captain Yannick Noah praised his two opening day victors, saying Pouille had again "dug deep" while Paire played a match "of his dreams."
The 2-0 lead for France means that the champions can book a place in back-to-back finals -- and the last in the competition's current traditional format — if Julien Benneteau and Nicolas Mahut prevail in Saturday's battle of 30-somethings in the doubles with Feliciano Lopez and Marcel Granollers. They seem on course for a rematch of football's World Cup final with Croatia in November.
The Croats lead the US 2-0 in the other semi-final. Paire had never been selected for his country in the 'World Cup of tennis' before, admitting himself that his explosive, erratic performances on court meant he could previously never properly be trusted.
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Yet he has grown into a much more reliable and consistent performer in 2018 which prompted Noah to select him for his first tie at the unlikely age of 29.
"I've waited a long time for this and it's a dream to win on my debut, hopefully it's not too late for me and I'll get more chances,” said Paire.
Playing with real flair and looking as if he was made for Davis Cup theatrics, Paire also showed real heart when struggling in the first set as he three times had to battle back from a set point down.
Paire, the world number 54, started with predictable unpredictability, delivering nine double faults in the opening set but after saving the set points with steel, the bearded shot maker was freed to play his most attractive tennis.
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