Lyles, who won the world 100-200m titles in Budapest last year, clocked a personal best of 9.81 seconds in the blue riband event at London Stadium.
It could not have been better timed, with the opening ceremony of the Paris Olympics just six days away.
"I'm going to win, it's what I always do. I'm getting faster every week," Lyles said.
In her own fine-tuning, world champion Bol set a new meet record of 51.30sec as she cruised to victory in the women's 400m hurdles.
"I am excited for Paris and of course to put on my best race there," she said, with world record holder and Olympic champion Sydney McLaughlin-Levrone in her crosshairs.
"I am looking forward to racing Sydney -- that will push us both. I will be ready for it and the relay as well of course."
Boost for Brits
There was a fantastic send-off to a raft of Paris-bound British athletes in front of a near sell-out crowd of 58,000 at London Stadium, the venue for the 2012 Olympics and home to English Premier League club West Ham United.
World and Olympic silver medallist Keely Hodgkinson just missed out on Caster Semenya's Diamond League record by blasting to a stunning victory in 1:54.61 in the women's 800m.
Perfectly led out by pacemaker Erin Wallace, the European champion was in total control of the race and came flying through the line in a meet record that improved her own British record.
"I just wanted to go for it and see what was there," Hodgkinson said.
"It was a little bit of bravery and fearlessness with a great atmosphere like this, I didn't want to waste the opportunity.
"I'm feeling really good and confident ahead of Paris."
Hodgkinson's British teammate Matthew Hudson-Smith might have sat out the European championships in Rome, but that didn't show as he bettered his own European record to 43.74sec in a scintillating 400m.
"Forty-three seconds before Paris is exactly what me, my coach and team were aiming for!" said Hudson-Smith.
"To get that world lead and to set myself up for Paris is what I really needed to show the rest of the world what I am capable of."
It did not all go totally to plan for home favourites as Dina Asher-Smith and Daryll Neita could only finish third and fourth in the 200m behind American winner Gabrielle Thomas -- in a meet record of 21.82sec -- and second-placed St Lucian Julien Alfred (21.86).
"It's made me feel confident going into the Paris Games after that one," said Thomas.
Aussies impress
There were three individual Australian winners at London Stadium: world champion Nina Kennedy claimed victory in the women's pole vault with 4.85m; Oliver Hoare claimed the men's mile in 3:49.03; and Mackenzie Little won the women's javelin in a personal best of 66.27m.
There was a surprise in the men's shot put, however, as Italy's European champion Leonardo Fabbri snatched a late victory with his fifth effort of 22.52 metres.
American favourite Ryan Crouser, who will seek a third successive Olympic title in Paris, finished second with 22.37sec.
"Overall I was pretty happy with today," said Crouser.
"Obviously I would have liked to win but I was pretty consistent out there so overall it wasn't a bad day.
"It was a good step in getting ready for Paris. I've got a couple more weeks but I can see myself rapidly improving after injury."
Nickisha Pryce of Jamaica proved her form with an impressive world lead of 48.57sec in the women's 400m, a personal best and meet record.
There was a further meet record in the non-Olympic distance of 3,000m, Switzerland's Dominic Lokinyomo Lobalu winning in 7:27.68.
With one eye on the Paris Games, Qatar's Mutaz Essa Barshim, who famously shared Tokyo gold with Italian Gianmarco Tamberi, was a late withdrawal from the men's high jump.
That was won by New Zealand's Hamish Kerr with a best of 2.30m.
