The happy couple held hands at the altar in the historic surrounds of St George's Chapel before exchanging vows in front of a star-studded congregation.
Harry, dressed in military uniform, appeared to say; "You look amazing...absolutely gorgeous," to his stunning bride during the ceremony.
They will take the titles of the Duke and Duchess of Sussex following their marriage.
Ms Markle's mother Doria Ragland cried tears of joy as her daughter entered the chapel in a wedding dress designed by Clare Waight Keller, artistic director at French fashion house Givenchy.
Harry arrived at the ceremony with his brother and best man, the Duke of Cambridge.
Ms Markle walked through the Nave of the stunning chapel on her own, followed by a procession of bridesmaids and pageboys.
She was met by Prince Charles at the start of the Quire, as her father has been forced to miss the event following heart surgery.
Tens of thousands of people waving union flags had earlier greeted Ms Markle as she was driven quickly along the Long Walk to the castle.
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Television star Oprah Winfrey, actor Idris Elba and Earl Spencer, the brother of Diana, Princess of Wales, were among the first guests to arrive for the wedding.
Actor George Clooney and his wife, the human rights lawyer Amal Clooney, soon followed - along with David and Victoria Beckham.
Among the first royal guests to arrive were the Princess Royal, the Countess of Wessex, princesses Beatrice and Eugenie and Zara Phillips and her husband Mike Tindall,
Ms Markle's former co-stars from TV drama Suits are also attending.
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The order of service, published on the morning of the wedding, revealed that Harry will wear a ring - not a given for royal men - and Ms Markle will not promise to obey her husband in the vows.
The moving soul classic Stand By Me by Ben E King was performed by Karen Gibson and The Kingdom Choir, with the gospel singers also performing Etta James's uplifting version of Amen/This Little Light of Mine - a favourite in African-American churches.
The presiding bishop of the American Episcopal Church, Bishop Michael Curry, gave a passionate address, saying: "There's power in love. Don't underestimate it. Don't even over-sentimentalise. There is power, power in love."
Approximately 600 guests are in the wedding congregation, including about 30 members of the Royal Family. They include the Queen and the Duke of Edinburgh, 96, who is well enough to attend after undergoing a recent hip operation.
Prince George is a pageboy, while Princess Charlotte is a bridesmaid.
In a moving tribute to Harry's late mother Diana, Princess of Wales, her sister Lady Jane Fellowes will give a reading during the ceremony.
On Friday evening, a relaxed-looking Harry said he felt "great" as he greeted well-wishers in a walkabout with his best man, the Duke of Cambridge, outside Windsor Castle.
The pair then headed to Coworth Park country house hotel in Ascot, where the prince spent the night away from his bride-to-be as is tradition.
Some 15 miles away, Ms Markle said she was feeling "wonderful" as she arrived with her mother Doria at the luxury Cliveden House Hotel in Taplow, Berkshire.
Prince Harry, 33, and Ms Markle, 36, became engaged following a whirlwind 16-month romance after going on a blind date in London.
She wed her first husband, film producer Trevor Engelson, in 2011 - but the pair divorced less than two years later.
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