Bolt defended his men's 100m title at London 2012, stunning the world as he won Sunday's final in an Olympic record time of 9.63 seconds.
The Jamaican sprinter went on to win a further two golds - in the 200m and 4x100m relay - before proclaiming: "I'm now a legend. I'm also the greatest athlete to live."
Meanwhile Kenyan middle-distance runner David Rudisha won gold in the men's 800m final and broke the world record with a time of 1.40.91 at London's Olympic Stadium.
Coe, a former middle-distance runner himself who scooped up four Olympic medals, including a gold each at Moscow 1980 and Los Angeles 1984, exclusively shares with Eurosport his high praise for Bolt and Rudisha.
'LONDON 2012 SAW BOLT TRANSCEND ATHLETICS'
"I think Bolt came of age in London. It wasn’t vintage Bolt if I am being completely honest, I think it was a bit closer than I think he probably thought, although he did power through quite literally. In 2008, that’s where he really burst on to the Olympics scene, the world records, then Berlin at the World Championships a year later.
"I think people recognised this wasn’t just a one off by the time he’d got to London and come through London, and he’d cemented himself as probably the biggest name of our sport of all time. We didn’t know what his form and fitness was going to be and he really was not particularly convincing during the heats.
"I remember him telling me about a conversation he had with his wonderful coach, coach Mills and he said to him before the race ‘stop thinking about it and just do what you were put on the planet to do’ and then he came through.
"The 200m was a slightly easier task for him. We’ve got great sprinters coming through, the one thing to remember and it’s quite a sobering thought for sprinters elsewhere in the world, but there isn’t a single record that Usain Bolt set at school level that hasn’t been broken in Jamaica.
"The question you always get is 'what was going to come after Usain?' The answer is 'you’ll never get another Usain'.
"When Muhammed Ali retired, you’re never going to get another Ali, but it doesn’t mean there you don’t get great boxers coming through, you’re going to get great sprinters. But are we ever going to have anybody that has dominated the landscape and gone so far in to transcending his own sport?
I can’t think of anybody in my lifetime that has had such a global reach in sport since Ali.
'RUDISHA DID WHAT HE SAID HE WOULD'
"I genuinely think David Rudisha’s performance in London was absolutely majestic, and Mo knows how hard it is to do what this guy did.
"In an Olympic final, he ran from gun to tape and didn’t put a foot wrong physically or mentally.
"I shared the most extraordinary conversation with the father of African distance running, Kip Keino, who said to me that he went down to the warm up track before the race, he saw the Kenyan team they had three in the final, and Kip turned to David and said, ‘what are you going to do?’
"Rudisha said, ‘I am going to break the world record and I am going to win the Olympic title’ and Kip turned to the guy that ended up finishing third in the race and said ‘what are you going to do?’ and he said ‘I am going to follow David’ and David turned around and said ‘don’t do that, because if you do, you will die’.
"Look, Mo has run Olympic finals, I have run Olympic finals, I doubt that we have ever sat there and thought about the time, if it takes us six days, you are only concerned about getting across the line before the next guy.
"To have somebody that had such presence of mind, such physical and mental certainty about what he was going to do that do.
He executed it in a way that I’ve never seen anybody execute an 800m and for me, that made him by a distance, the best 800m runner of all time and I say that through gritted teeth.
You can watch Return to London 2012 on Eurosport 2!
Saturday 30th May (2pm, replayed at 7pm) will give viewers the chance to relive the iconic night of the games – known ever since as Super Saturday.
On a memorable night at the Olympic Stadium, Team GB secured three gold medals with Greg Rutherford, Dame Jessica Ennis-Hill and Sir Mo Farah all topping the podium. Greg and Mo will look back on the historic evening and discuss some of the other seminal moments. Seb Coe and Tony Minichiello also join the chat.
Sunday 31st May (midnight) will see the week come to a close with Boyle’s equally impressive Closing Ceremony to book-end a celebratory period in the country’s sporting history.