Jayasurya made his debut in 2001 in the Malayalam film Dosth as a junior artist. Oomappenninu Uriyadappayyan (2002) was his breakout role. He was able to make a mark for himself in the industry with performances in films such as Swapnakkoodu (2003), Pulival Kalyanam (2003), Chathikkatha Chanthu (2004), Classmates (2006), Arabikkatha (2007), Shakespeare M.A. Malayalam (2008), and Gulumaal (2009). By the 2010s, Jayasurya had started acting in more drama-centric roles with films such as Cocktail (2010), Beautiful (2011) and Trivandrum Lodge (2012), in which have been critically acclaimed.
Jayasurya has acted in several films in Malayalam and Tamil. Jayasurya became popular among family audiences as an anchor in musical programs on Malayalam television.’Jagathy Vs Jagathy’ (Surya TV) is one of the famous show he done during early stages. He also played minor roles in films. Notable among these was the comedy artist in Aparanmar Nagarathil.