The 22-year-old American won balance beam and floor gold on Sunday to make it 25 medals at the global competition in Stuttgart
This time, the 22-year-old American has become the most decorated gymnast in World Championships history with 25.
After Saturday's competition where she won the gold medal on the vault, she was tied with Vitaly Scherbo on 23. Now, she owns the record outright.
The historic 24th medal came on the balance beam where she took gold ahead of defending champion Liu Tingting and fellow Chinese Li Shijia.
An hour or so later, she clinched her fifth gold medal of the week, easily taking the title on the floor. That took her tally to an unprecedented 19 world titles and 25 medals overall.
Though Biles has twice before won the world title on the balance beam, she has struggled to erase the memory of an error in the Rio 2016 beam final which dropped her to third.
Last year, she dropped off the beam on a front flip with a half twist during the women's all-around final.
But in Stuttgart, she has owned the beam, posting the top score in all four rounds: qualifying, the team and all-around finals and Sunday's apparatus final. She credits the turnaround to balance beam coach and 1996 Olympian Cecile Landi.
"It means the world [that Cecile is here]," Biles said earlier this week, referencing that Cecile Landi has often stayed home while husband, Laurent, handles competition duty. "Cecile has definitely helped a lot bringing back that confidence because after Rio kind of trashed myself and my beam work."
As Biles' massive 15.066 went up on the scoreboard in the arena, reflecting a nearly flawless routine, she leapt from her seat in the 'kiss and cry,' punching the air with joy before giving a high five to Laurent Landi as she broke her tie with Scherbo for most World Championship medals.
The score also saw her become the first gymnast to break the 15.000 mark on balance beam at the World Championships since the last Olympics.
"I was really excited," she said. "I thought it was gonna be at least 14.8, 14.9, but to see 15, I was like well that's pretty crazy, so I was very proud."
Liu earned a 14.433 with Li at 14.300.
Biles made it five in the floor exercise, the discipline she has dominated more than any other.
The champion from 2013, 2014, 2015 and 2018 made it five World Championship triumphs to go with her Olympic floor gold.
She did it in style, nailing her triple-double - known as the Biles II - on her way to a score of 15.133, a full point clear of her rivals.
"Honestly, I just couldn't move. I was so tired," Biles said of the moment she took to hold her final pose on centre stage after closing our her historic Worlds performance.
"I was just like I'm going to stay here because if I come back I'm literally going to be breathing like a dog." - Simone Biles on holding her pose at the end of her winning floor routine
It completes a record gold haul at a global event for Biles who goes home with five golds, one more than she managed in 2014, 2015 and 2018 and at Rio 2016.
Team-mate Sunisa Lee took silver with Russia's Angelina Melnikova claiming bronze.
"I think with every year it gets easier and easier to compete. I feel myself more confident, I grow in my programs, I feel that I am becoming stronger," said Melnikova who stars in the Olympic Channel original series 'All Around'.
"I really worked a lot before these World Championships and I am happy that I could show my work here."
In the first final of the day, Russian's Nikita Nagornyy and Artur Dalaloyan repeated their 1-2 finish from the men's all-around, taking gold and silver, respectively, in the men's vault final. For Nagornyy, it was his third gold medal of the championships.
The British continued their individual apparatus finals success Sunday.
One day after Max Whitlock regained his pommel horse world title and both Becky and Ellie Downie picked up their first individual world medals, Joe Fraser became the first Briton to win the gold on the parallel bars. It was also the first medal of any colour for Team GB on the event.
Already in tears when it became clear he was assured of a medal, all of Fraser's teammates found their way to the field of play as the final score was posted. Embracing at first, they then lifted Fraser up, throwing him up and down in delight.
The 20-year-old from Birmingham joins Whitlock and Beth Tweddle as Britain's only gymnastics world champions.
Fraser said, "It still hasn't sunk in, still hasn't sunk in. I think it might take a few weeks, maybe months.
"For now, I'm just ecstatic with the way I've performed out there... and to be in the company of such great, great gymnasts that I've looked up to for my whole junior career and to be put up there with the likes of Max and Beth, I can't comprehend how proud I am."
Ahmet Onder took silver to secure Turkey's second world medal a day after Ibrahim Colak captured still rings gold. Japan's Kazuma Kaya completed the podium.
In the final event of the week, the high bar final, Brazil's Arthur Nory Mariano claimed the title to secure his first World Championship medal.
As with Fraser's title on the parallel bars, Mariano's victory was his country's first medal on that piece of apparatus.
Croatia's Tin Srbic took silver with Dalaloyan rounding out the podium for his second medal of the day.
Mariano famously wept with joy alongside compatriot Diego Hypolito after they took bronze and silver respectively in the floor final at Rio 2016.
He cried again in Stuttgart but said afterwards, "I think it was a different emotion in Rio. I was in [front of] my hometown crowd in Brazil so my family was there. I did not expect it too much because I was the ninth into the floor final, and I don't know I had to do harder routine and was very, very emotional in Rio.
"Now, I am working, working so hard to be in that final, and to win the gold so it's different, but it's amazing, still an amazing feeling."