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2019: Australian Open semifinal, top 25 debut, Wimbledon doubles quarterfinal

Her rise continued at the Australian Open. Prior to the tournament, she had never won a match at a major event. After upsetting 14th seed Julia Görges in a tough first-round match, Collins won her next three matches in straight sets; first against Sachia Vickery, then against 19th seed Caroline Garcia. In the round of 16, Collins pulled off the biggest upset of the tournament, dominating the second seed and three-time major champion Angelique Kerber, in straight sets. She thus reached the quarterfinals, where she defeated Anastasia Pavlyuchenkova in three sets. In the semifinals, she lost to eighth seed Petra Kvitová, in two sets.[13] Collins rose to a career-high ranking of No. 23 on 28 January 2019, following the tournament.

She also recorded wins at all the other Grand Slam events, reaching the second round at the French Open and US Open as well as the third round at Wimbledon. She achieved her best-ever Grand Slam doubles result at Wimbledon, reaching the quarterfinals with Bethanie Mattek-Sands. Collins struggled outside of the majors though, reaching the quarterfinals at just one tournament (the Charleston Open). In December, she won the Hawaii Open, an exhibition tournament, upon the withdrawal of her finals opponent Angelique Kerber. Collins finished the year ranked World No. 31.

At the end of 2019, Collins revealed that she was suffering from rheumatoid arthritis,[14] similar to Carolina Wozniacki.

2020: French Open quarterfinalist

Collins began 2020 with three wins over top-15 opponents. She defeated world No. 5, Elina Svitolina, 6–1, 6–1 in the first round at the Brisbane International before falling to world No. 13, Madison Keys, in straight sets in the quarterfinals. The following week at the Adelaide International, she defeated No. 15, Sofia Kenin, 6–3, 6–1 in the second round, and then No. 7, Belinda Bencic, 6–3, 6–1 in the quarterfinals. Collins fell to world No. 1, Ashleigh Barty, 6–3, 1–6, 6–7(5–7) in the semifinals.[15] However, she lost in the second round to Yulia Putintseva at the Australian Open, and dropped outside the top 50 due to failing to defend her semifinalist points.

Due to the six-month shutdown of the WTA Tour caused by the COVID-19 pandemic, Collins did not play again after the Australian Open until August. She lost in the opening round of her first two tournaments back, to Jil Teichmann at the Western & Southern Open and Anett Kontaveit at the US Open. However, Collins rebounded at the French Open, where she reached her second career Grand Slam quarterfinal. Along the way, she upset two-time Grand Slam champion and former world No. 1, Garbiñe Muguruza, in the third round (handing the Spaniard her earliest exit from Roland Garros since 2013) as well as 30th seed Ons Jabeur, both in three sets. Her run ultimately came to an end against compatriot and reigning Australian Open champion Sofia Kenin, in a match that for both players was their fourth three-setter of five matches.

Danielle Collins was sidelined for the first half of the season with debilitating pain in her back. She was diagnosed with endometriosis and proceeded to have a "tennis-ball sized" cyst removed. In addition to that surgery, Collins was also taking medication for rheumatoid arthrisis.