Alfred coasts in London, but Lyles pipped in season-opening 100m
Alfred, the women's 100m Olympic champion, set a meet record with a world-leading 21.71 seconds at a 60,000-capacity sell-out London Stadium.
It put her joint ninth on the all-time list for the 200m in a massive boost for the St Lucia sprinter before the world championships in Tokyo in September.
"It was a strong first 150 metres of the race and I managed to control it to finish strongly," said Alfred, whose 100m gold at the Paris Olympics was the first of any colour for her tiny Caribbean island homeland.
"It was a great race for me, and races like this give me a lot of confidence as we get closer to Tokyo. I did the 200m last year before the Olympics and I finished second, but seeing how I ran today and how comfortable I felt, I am a lot more confident in my 200m heading into the worlds," she added.
Lyles, who won Olympic gold in the men's 100m in Paris last year, suffered a dreadful start and was left chasing Jamaica's Oblique Seville, who racked up a straightforward gun-to-tape win in 9.86sec.
The 28-year-old American, making a late start to the season after coming back from an ankle tendon injury, insisted, however, that he felt great.
"I feel extremely healthy and I am feeling no pain," he said.
"I wanted the win but I think it was my fastest ever season opener, so I will take that result today."
In an afternoon of high-class track and field, Femke Bol produced yet another dominant run in the 400m hurdles for her 29th consecutive Diamond League win.
The Dutch athlete clocked 52.10sec, finishing a full second ahead of American Jasmine Jones.
"I wanted to run quicker in Monaco but my second bend was really not great there," Bol said, referring to her world-leading 51.95sec from last week.
"I had hoped to do better here. I think I executed the second bend better here but other elements were a little less good, so it is a bit disappointing."
- Wanyonyi still chasing Rudisha -
Kenya's Emmanuel Wanyonyi, hunting down compatriot David Rudisha's 800m world record of 1:40.91 -- set when he won Olympic gold in this same stadium in 2012 -- fell short.
Wanyonyi, the current Olympic champion, edged Canada's Marco Arop for victory in a meet record of 1:42.00.
"My training right now is at 80%, so I will be upping the training in the next few weeks and over the next races before Tokyo," the Kenyan warned.
There was also a meet record of 3:28.82 for Kenya's Phanuel Kipkosgei Koech in a loaded men's 1500m.
Reigning world champion Josh Kerr came second in 3:29.37 in a dramatic final event at the home of Premier League club West Ham.
Olympic 1500m bronze medallist Georgia Hunter Bell delighted the home crowd by producing an impressive kick to win the women's 800m in a season's best of 1:56.74.
It was the first of a trio of wins by British athletes in quick succession.
Charles Dobson ran a personal best of 44.14sec to seal a dramatic victory in the men's 400m, overhauling fellow Britain Matthew Hudson-Smith, the world and Olympic silver medallist, in the final metres.
"It is an incredible feeling, I love running here in front of a massive home crowd. It is just awesome to get that time," said Dobson.
"Tactically it went perfectly, and I won the race, so what more can I ask for?!"
And Morgan Lake claimed an unlikely win in the women's high jump, the sole athlete to clear 1.96m to finish ahead of the likes of Australia's 2022 world champion Eleanor Patterson and Ukraine's Yaroslava Mahuchikh, the world record holder and current world and olympic champion.
The outstanding performance in the field came from Lithuania's world record holder Mykolas Alekna, who threw a Diamond League and meet record of 71.70m in the men's discus.
Ethiopia's Gudaf Tsegay also set a meet record of 4:11.88 in an electric women's mile, bettering the previous best set by Sifan Hassan in 2018 by almost three seconds.
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