The 22-year-old son of former tennis great Liz Smylie finished in a tie for second at Royal Cinque Ports in Deal, England, to become the sixth Australian in the field for The Open, which begins on July 18.
The Queenslander shared the first-round lead after posting a five-under 67, but fell away with three front-nine bogeys in the final round.
The left-hander recovered one stroke after the turn to finish on 74, his three-under total keeping him safely inside the top four and earning an Open invite.
Twelve Australians played across four venues in a bid to earn a coveted place at Royal Troon, but Smylie was the only qualifier.
He'll join the in-form Min Woo Lee, along with Adam Scott, Jasper Stubbs, Jason Day and 2022 Open champion Cameron Smith in the field.
Congratulations to Matthew Southgate, Elvis Smylie, Jaime Montojo and Luis Masaveu who have today qualified for The 152 Open Championship at — Royal Cinque Ports Golf Club (@RCPgolfclub) @RoyalTroonGC through Final Qualifying at Royal Cinque Ports. pic.twitter.com/iACY6CSBXZJuly 2, 2024
The Southport talent has been knocking on the door of a maiden title since turning professional three years ago.
"Just saying that I've qualified for The Open gives me goosebumps," he said.
"The last time I went to The Open was at Royal Troon in 2016, when I was 14 years old.
"Going there as a spectator eight years ago and now going back as a competitor ... I don't know what to say. I just can't wait for the experience."
Smylie said his father Peter was booking flights to join him while his mother, a winner of three mixed and one women's doubles grand-slam titles, was already in the UK on Wimbledon commentary duties.