In the following week, Barrios qualified for his first Grand Slam at the 2021 Wimbledon Championships, where he lost to former finalist Kevin Anderson in the first round.

In the following month, Barrios won his first Challenger title in Meerbusch, Germany, defeating Juan Manuel Cerúndolo in two sets at the final.

He reached the quarterfinals at the 2023 Córdoba Open as a wildcard defeating Daniel Galan and eight seed Bernabé Zapata Miralles.

[8] After qualifying for the main draw, he won his first Major match against Sebastian Baez at the 2023 Wimbledon Championships,[9] before losing to David Goffin in the second round.

[10] He made his debut at the 2024 United Cup in mixed doubles partnering Daniela Seguel where they stunned Greek top 10 duo Maria Sakkari and Stefanos Tsitsipas.