Smith, who was the league's equal leading goalkicker in 2024, got her wish to head to the Swans on Wednesday during a complicated deal that also involved Hawthorn.
The 25-year-old, who played one game for Gold Coast, made 76 appearances for the Lions after joining them in 2021.
Smith played in the club's 2021 and 2023 premierships and was named All-Australian in 2024.
She will feature in a powerful forward line at the Swans with superstar Chloe Molloy.
Sydney are still looking for a new coach, after parting ways with Scott Gowans when the Swans blew an opportunity to make this year's finals.
"We really rate Taylor as a player and a person and we feel she will add a lot to our squad," Swans AFLW football boss Amanda Turner said.
"Having played a key role in two premierships, she knows what success looks like and she will complement our existing playing group really well.
"Over the last couple of seasons, Taylor has established herself as one of the AFLW's best forwards and we think she can have an immediate impact for us next season."
Smith joins Ellie Hampson (Port Adelaide) and Poppy Boltz (GWS) in exiting the Lions after their grand final thumping to North Melbourne last month.
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