The Jamaican sprinter kicked off the second half of the Games in style, setting an Olympic record and taking gold in the men's 100 metres in 9.63 seconds.
He was slow out of the blocks but once he got his giant stride going he was unbeatable once again, leaving compatriot Yohan Blake and 2004 Olympic champion Justin Gatlin in his wake with the second-fastest time in history.
"I knew it was going to be like this. There wasn't a doubt in my mind it was going to be like this," Bolt said after finishing just .05 of a second outside his world mark.
Earlier, another big day from the Brits was the talk of the town in London.
Andy Murray beat Roger Federer for the men's singles tennis gold, gaining a measure of revenge for the Wimbledon final he lost on the same Wimbledon court to the Swiss star a month ago.
And he didn't mess around, dominating a listless Federer 6-2, 6-1, 6-4 Sunday, by winning nine consecutive games at one stage and breaking the seven-time Wimbledon champion's serve four times in a row.
"It was the biggest win of my life," said an emotional Murray. "I've had a lot of tough losses in my career. This is the best way to come back from the Wimbledon final. I'll never forget it."
The Scotsman couldn't add to the British gold medal total when he and Laura Robson lined up in the mixed doubles final. The gold went to Max Mirnyi and Victoria Azarenka of Belarus, who won 2-6, 6-3, 10-8 to leave the British pair with silver medals.
Later, Ben Ainslie won his fourth straight gold medal and fifth Games medal overall, making him the most successful sailor in Olympic history.
Ainslie, who trailed most of the event until Sunday's final race, eclipsed Denmark's Paul Elvstrom as the most successful sailing Olympian. Elvstrom won four straight gold medals from 1948-60, including three in the Finn class.
"It is always hard when people say you are a 'dead cert' to win," Ainslie said. "You try to tell them that is not the case, but they don't listen."
The two new golds Sunday gave Britain 16 — with eight of them claimed over the weekend. That's good enough for third place in the gold medal race behind the United States and China.
Canada is still 11th overall in the overall medal standings with 10 — one gold, three silver and six bronze. The Canadian team will try for more on Monday when the individual and team equestrian medals are awarded.