"This evening, 56 years after the Apollo 11 moon landing, I spoke with the astronaut Buzz Aldrin," the American pope wrote on X.
"Together we shared the memory of a historic feat, a testimony to human ingenuity, and we reflected on the mystery and greatness of Creation", he wrote.
After Neil Armstrong, who died in 2012, Aldrin was the second person to set foot on the Moon on the historic Apollo 11 mission that secured the United States' victory in the space race.
A devout Christian, Aldrin took communion on the lunar surface using a travel kit provided by his Presbyterian pastor.
The pope said he blessed the 95-year-old US astronaut and his family during the call.
Earlier Sunday, Leo visited the Vatican Observatory, which sits on a leafy hilltop near the papal summer home of Castel Gandolfo.
Vatican photographs showed the pope looking through a large telescope in the Observatory, one of the oldest astronomical research institutions in the world, where planetary scientists mix the study of meteorites with theology.
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