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The duo originally set a world record in 2016 when they climbed 90 stairs of the cathedral in 52 seconds.
Guinness World Records proposed adding 10 more steps this time and the Vietnamese duo agreed to take on the new challenge.
Both artists left Vietnam for Spain on December 17 and spent several days training before the contest.
Strict COVID-19 prevention measures adopted by the Spanish Government, including the closure of fitness clubs, affected their training. The two artists had to train and perform in freezing temperatures.
But their efforts paid off when the artists finished climbing up 100 steps in 53 seconds.