He was also praised for his supporting roles in Wide Awake (2007) and Moss (2010), and gained newfound popularity in 2012 because of the TV drama My Husband Got a Family.

[10] He gave a memorable supporting turn as a cynical prosecutor in 2010's Moss, the blockbuster mystery film based on a popular online comic series.

The drama was a big hit, it not only consistently topped its timeslot throughout its long run, but ranked number one on the 2012 yearly TV ratings chart.

[21][22] As a result, Yoo enjoyed his biggest surge of mainstream popularity since his debut, landing commercial contracts and gaining the nickname "Nation's son-in-law".

Yoo said he began writing diaries back in university when his professor recommended that he try filling up at least one journal each year with personal reflections.

The book contained highlights from his 20 years of journaling life—from his days as a college student, moments on the set of several productions to his travels and vacations—as well as poems and sketches made by the actor in his everyday life.

[24] For the aerial action blockbuster R2B: Return to Base, Yoo along with the rest of the cast had to undergo months-long physical training for their role as jet fighter pilots.

The actors also had to pass mandatory tests for actual pilots to be able to get into the cockpit—in a low-pressure chamber, emergency escape routine, simulated flight as well as training to develop tolerance for acceleration.

[28] On December 19, 2013, he released his first album, titled Junes; besides singing, Yoo composed, wrote the lyrics and produced all the seven songs included.