Raai Laxmi made her debut at the age of 17 in the Tamil film Karka Kasadara in 2005, after the director R. V. Udayakumar had been impressed with her performance in a short film titled Valmiki. Subsequently, she appeared in a number of Tamil films, including the comedy film Kundakka Mandakka (2005) opposite R. Parthiban, Perarasu’s action-masala flick Dharmapuri (2006), and the romance film Nenjai Thodu (2007). In 2008, she began working in more serious films such as the drama film Velli Thirai, in which she played herself, and the action thriller Dhaam Dhoom directed by Jeeva. She received positive feedback for her portrayal of a lawyer in the latter. A review from Behindwoods wrote: “The latter (Raai Lakshmi) sizzles even as she is supposed to play the court professional who is caught in the web of smuggling drugs”. She won her first Filmfare Award nomination in the Best Supporting Actress category.
She made her debut in Malayalam in 2007, starring in Rock & Roll opposite Mohanlal. She followed it up with several successful films such as Annan Thambi, 2 Harihar Nagar (2009), Evidam Swargamanu (2009) opposite Mohanlal, and Chattambinadu (2009) opposite Mammootty. She appeared in three Tamil films in 2009, Muthirai, Vaamanan and Naan Avanillai 2.
In Vaamanan, she played a glamorous supermodel. In 2010, she was seen in three films. She made special appearances during song sequences in two of them, In Ghost House Inn and Pen Singam and portrayed a cowgirl in the Tamil film Irumbukkottai Murattu Singam.