However, it was 24-year-old Vondrousova who secured the crucial break at 4-4 when a baseline rally ended with Pegula sending a backhand long.
The twists and turns kept coming, though, as Pegula began finding her range in the second set.
In the decider, momentum looked to be staying with the 29-year-old Pegula as she saved three break points in the first three games and then broke Vondrousova by forcing her long.
I just wanted to stay as long as I could and fought until the end and I'm just so happy.
For Pegula, it was another quarter-final heartbreak, having never gone beyond the last eight at a Grand Slam.
Persons:
Marketa Vondrousova, Jessica Pegula, Hannah Mckay LONDON, Ukraine's Elina Svitolina, Pegula, Vondrousova, Vondrousva, Zheng Jie, Barbora, Christian Radnedge, Ken Ferris
Organizations:
Lawn Tennis, Croquet Club, U.S, REUTERS, Wimbledon, Thomson
Locations:
London, Britain, Czech, Poland