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He was then cast in the KBS sitcom The Sound of Your Heart, based on the webtoon of the same name. In 2016, Lee starred in tvN's Entourage, a South Korean remake of the American series. The same year, he was appointed ambassador of the "2015 Korea Brand & Entertainment Expo" and received commendation from the trade minister for boosting the Korean Wave industry.
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The one-act play was aired on January 1, 2016. He also starred in the two-episode drama Puck!, where he played a loan shark who joins a college ice hockey club. Collective Invention was screened in the Vanguard section of the 2015 Toronto International Film Festival, marking Lee's first red carpet appearance at an international film festival. In 2015, Lee played the protagonist in Collective Invention, whose condition is caused by side effects from a newly introduced drug. Lee and Hwang Chansung (of boyband 2PM) then starred in the film A Dynamite Family, about five bickering brothers living in the village of Deoksu. He then returned to television with the medical melodrama It's Okay, That's Love, playing a patient suffering from Tourette syndrome, a neurological disorder characterized by repetitive, stereotyped, involuntary movements and vocalizations called tics. The neo-noir film is about three friends (played by Ji Sung, Ju Ji-hoon, and Lee) whose friendship gets destroyed after getting involved in a murder case. In 2014, Lee played his first major role on the big screen in Confession. He held another one in Malaysia on January 4, 2014, attended by almost 3,000 fans. Attended by 2,000 fans, it was considered a success. On August 17, 2013, Lee held his first solo fan meeting of his career in Singapore. While filming Goddess of Fire, he participated in an energy conservation campaign alongside child actress Kim Yoo-bin. He was then cast as Prince Imhae (villainous brother to King Gwanghae) in the 2013 period drama Goddess of Fire.
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Lee had publicly stated that he wanted to play an antagonist in TV or film.
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In 2013, after another supporting role in A Wonderful Moment, Lee voiced the lead character Marco in the animated movie Maritime Police Marco, opposite fellow Running Man regular Song Ji-hyo, who voiced for Lulu. Later in the year, he reunited onscreen with his former Running Man co-star and real-life best friend Song Joong-ki in the TV melodrama The Innocent Man. In 2012, Lee played supporting roles in the romantic comedies Wonderful Radio and All About My Wife, and thriller The Scent. In 20, Lee won back-to-back awards at the SBS Entertainment Awards for "New Star Award" and "Best Newcomer in Variety", respectively. Lee's popularity increased after joining SBS' Good Sunday variety show Running Man, gaining the nickname "Prince of Asia" due to his large number of overseas fans. He made his acting debut in the 2008 sitcom Here He Comes, which was followed by High Kick Through the Roof. Lee began his entertainment career as a model in 2007. Lee was born on Jin Namyangju, Gyeonggi, South Korea.