The 23-year-old has signed a three-year contract with the club until the summer of 2029.
Hailing from Peckham, and a graduate of the Arsenal and Chelsea youth systems, Lloyd-Smith began her professional career at Charlton Athletic, before a spell at the highest level of collegiate football with the University of South Alabama.
The forward joined Southampton in July 2022 and registered her first goals for the Saints just two months later, scoring a brace against Palace at Selhurst Park.
Lloyd-Smith then signed for Bristol City in 2024, where she would go on to score 23 times in 48 appearances for the Robins.
She was the top scorer in the Barclays Women’s Super League 2 last season, with an impressive strike rate of 11 goals in 21 appearances – including a final-day hat-trick against Sheffield United.
Lloyd-Smith also plays for England U23s and came on as a substitute in April's final win over Sweden, as the Young Lionesses were crowned as the 25/26 U23 European Competition champions.
Lloyd-Smith said: “It’s almost like it was meant to be – I’m happy to be back in South London, back at home.
“I know I’m going to be playing for something more now – my roots, where I’m from. I'll always be proud to be from Peckham. It means everything.”
Manager Jo Potter added: “Lexi is a real talent, who showed us all what she could do in the WSL2 last season.
“Her speed and finishing will be huge for us in the top-flight.”