Jayasurya began his career as a mimicry Artist and hosted a few television shows on Malayalam channels. He made his acting debut as a background actor in the 1999 film Pathram. His break-through was playing a mute in Oomappenninu Uriyadappayyan (2002). In the 2000s, Jayasurya was popular for his comic-oriented roles in Swapnakkoodu (2003), Pulival Kalyanam (2003), Chathikkatha Chanthu (2004), Chocolate (2007) and Gulumaal (2009), and at the same time villain roles in Classmates (2006), Arabikkatha (2007), and Kangaroo (2007). By the 2010s, Jayasurya gained critical acclaim for his roles, in films such as Cocktail (2010), Janapriyan (2011), Beautiful (2011), Trivandrum Lodge (2012), Apothecary (2014), Iyobinte Pusthakam (2014), Lukka Chuppi (2015), Su.. Su... Sudhi Vathmeekam (2015), and Captain (2018). He was also popular for comedy films, such as Punyalan Agarbattis (2013), Amar Akbar Anthony (2015), Aadu (2015) and Aadu 2 (2018). Jayasurya made his debut as a Producer by co-producing the film Punyalan Agarbattis and is also credited as playback singer in a few films.