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It was their first official engagement since they were last seen at Remembrance Day services in November.
During their visit, the couple toured the Canada Gallery and viewed a special exhibition by indigenous Canadian artist Skawennati, an award-winning new-media artist based in Montreal.
The Duke and Duchess also met different members of the High Commission team who work in a range of sectors supporting the partnership between Canada and the UK.
The Sussexes last visited Canada House on Commonwealth Day last March, when they met and spoke with young Canadians from a wide range of sectors including fashion, the arts, business and academia, about their experiences as expats as well as opportunities for young people working in the Commonwealth.
The Duchess, particularly, has strong ties to Canada, having lived and worked in Toronto whilst starring in the US television drama Suits.
The couple were first pictured together in the city when she joined her then-boyfriend, Prince Harry, at the 2017 Invictus Games.
They are expected to have a busy few months as they formally launch their own charitable foundation.