Sebastian Coe applauded Britain's athletics heroes and said their performances were "sensational".
Jessica Ennis led the way with heptathlon gold, and was followed to Olympic titles by Greg Rutherford in the long jump and Mo Farah after a gutsy sprint finish in the 10,000 metres.
"I think we've witnessed something sensational," said Lord Coe, chairman of Games organisers LOCOG and a two-time former 1,500 metres track gold medallist.
"I've never known a night in UK athletics like that, it was unbelievable."
He said it must be considered one of Britain's greatest ever days in sport, with the team also securing two golds in rowing and another in cycling.
"I think it has to be up there," Coe said.
And Coe confirmed he was on the point of tears as he presented Ennis with her gold medal. Like Ennis, Coe was brought up in Sheffield.
Asked if there was a tear in his eye, Coe said: "Yes, probably. She's a Sheffield girl, same athletics club. I know the city very well, it's just a fantastic moment for Sheffield."
Coe believes such evenings can prove inspirational, helping towards the legacy objectives on which London's bid for the Games was founded.
"We've really got to build on that," he said. "This isn't going to be a case of 'We've had a fantastic Olympic Games and it'll happen without further management', but this is the best opportunity any of us will have in our lifetime to get more young kids into sport."
The frenzied crowd in the 80,000-capacity stadium went wild as Ennis, the poster girl of the London Games, won the 800m with a sprint finish, crowning two days of tough competition in the heptathlon.
In front of spectators including the Duke and Duchess of Cambridge, Olympic silver medalist Zara Phillips and Prime Minister David Cameron, Ennis wept as she stood on the podium to receive her gold medal.
She said: "I can't believe I've had the opportunity to come to my first Games in London and won an Olympic Gold medal. It's unbelievable."
Former sports minister and ex-Sheffield MP Richard Caborn, who was in the stadium with his family, said: "She's our golden girl. She's stuck with Sheffield and Sheffield's stuck with her."
Her first coach, Mick Thompson, said: "You can't get better than this. Where does she go next?"
Rutherford was the next athlete to claim victory for Team GB, with a surprise gold medal in the long jump. He described his victory as the "most amazing feeling in the world".
He was followed by Farah who danced for joy around the track after winning the 10,000m, hailing it as "the best moment of my life".
The performances in the Olympic Stadium topped off a day which also saw a sensational world record-breaking performance by women cyclists in the frenzied atmosphere of the velodrome which led to another gold in the team pursuit.
The team of Dani King, Laura Trott and Joanna Rowsell led from the start to beat the US in a world record time of 3:14.051.
And earlier, at Eton Dorney, an ecstatic crowd cheered the men's coxless four of Andrew Triggs Hodge, Pete Reed, Tom James and Alex Gregory to a victory, which extended Britain's dominance in the event to 16 years.
This was followed just minutes later by Kat Copeland and Sophie Hosking claiming gold in the lightweight event.
It was the best day for gold medals since 1908 with Team GB now boasting 14 gold, seven silver and eight bronze and in third place after China and the US.
Which of Team GB's athletics golds did you enjoy the most?