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2010-2014

He finally made his debut in 2010's Prosecutor Princess in that same year also appeared in his first film role in the horror movie Ghost. Later that year he got a supporting role in the popular series, Secret Garden where he played a talented composer who was gay and had a romantic interest in Oska, played by Yoon Sang Hyun, an extravagant Hallyu singer who was the second lead in the highly rated drama. He started to gain further traction in his career when he appeared in High Kick 3: The Revenge of the Short Legged the following year, in 2012 he got his breakout role by appearing as a high school student in the teen drama series School 2013 where he received huge accolades for his acting in that drama, that opened the way for him to appear in one of 2013's top-rated dramas I Hear Your Voice, He starred as the lead Park Soo Ha, an intelligent young man who could read minds. He also continued to appear in movies that same year such as No Breathing and The Face Reader both turning out to be box-office hits.

In 2014 he acted in the film Hot Young Bloods with Park Bo Young, which is set in a farming village in Chungcheong back in the 1980s and focuses on the lives and loves of several high school students. It is Jong Suk's second film in the lead role and he again plays a high school student who is a cheesy womanizer. He also appeared in the drama Doctor Stranger the drama was a huge success in the Chinese market, he appeared next in the drama Pinocchio opposite actress Park Shin Hye, both actors received huge accolades for their roles and the drama was also a huge success nationwide and worldwide.

2015-onwards

In December 2015 he was confirmed as part of a new historical drama television series directed by Jin Hyuk, a Chinese Korean co-production entitled Jade Lover which takes place in 1930 and whose filming began in January 2016 in China. It was also announced he would starred specifically as the lead opposite Chinese actress Zheng Shuang in said historical drama television series. In July 2016 Lee Jong Suk appeared once more in South Korean small screens as the lead of W alongside Han Hyo Joo it was a successful drama.

In 2017, he starred in the film VIP in his first villain role, the movie was a success but it had its fair share of controversy over its depiction of brutal and violent scenes against women. In that same year co-starred with Bae Suzy as the leads of the supernatural-procedural drama While You Were Sleeping. The drama was also a huge success and he received high accolades for his performance.

In March 2018 it was announced that he had joined the main cast of the new two-part miniseries Hymn of Death where he will bring playwright Kim Woo-jin to life. At the end of September of the same year it was announced that he had joined the romance and comedy series Romance Supplement (also known as "Romance Is A Supplement") where he will bring to life Cha Eun-ho, a brilliant writer who is also the company's youngest editor-in-chief.