Dressed in a sober navy suit and dark striped tie, the prince, 29, was smiling and relaxed in a brief meeting with President Michelle Bachelet at the ornate La Moneda palace in the capital Santiago.
Earlier in the day, he laid a wreath at a monument of Bernardo O'Higgins, who helped free Chile from Spanish rule, and was later scheduled to visit a kindergarten and attend a function to celebrate the official birthday of his grandmother, Queen Elizabeth II.
The sports-mad Harry arrived in Santiago yesterday night on a scheduled flight after an official visit to Brazil, where he saw the England football team play out a 0-0 bore draw against Costa Rica on Tuesday in their last game of a disappointing tournament.
The prince recently made headlines with his party-going antics at a wedding in Memphis, and there has been intense speculation about his private life after his split from blonde girlfriend Cressida Bonas.