Yook achieved his breakthrough when he landed a leading role in the teen drama Who Are You: School 2015, alongside Kim So-hyun and Nam Joo-hyuk. He also released an OST for the show, "Love Song" with Park Hye-soo. After the series ended, he experienced a rise in popularity and landed several endorsement deals. Yook then starred in the horror mystery series The Village: Achiara's Secret alongside Moon Geun-young in 2015. He received the "New Star award" for his performance in The Village: Achiara's Secret, and won "Best Couple award" with Kim So-hyun for Who Are You: School 2015.
In 2015, Yook joined King of Mask Singer, competing under the alias Tired Bumblebee, and received good feedback for his performance. He was paired up with Red Velvet's Joy in the fourth season of reality show We Got Married. The couple went on to release a duet titled "Young Love", with the pair contributing to the lyric composition of the song with the help of his bandmate BTOB's Im Hyun-sik as the producer. At the 2015 MBC Entertainment Awards, Yook received the "Best Couple award" alongside Joy and the "Best Male Rookie (in Variety) award". The couple departing from We Got Married on May 7, 2016.
In September 2015, Yook became one of the trio main hosts Yook Sungjae-GOT7's Jackson Wang-and actress Kim Yoo-jung of the music-program Inkigayo and left the show in May 2016. In 2016, Sungjae was appointed as an ambassador of the King Sejong Institution. He also became part of BTOB's first sub-unit, BTOB Blue, and debuted in September 2016.
In 2015, Yook took part in a fundraiser that auction items to the Social Welfare Community Fund for Love to support low-income children. In December, 2015, SBS revealed that Yook donated ₩3 million to Jeonbuk National University Hospital, which was the filming location of The Village: Achiara's Secret. The same year, he also participated in Briquette Sharing Campaign of the Korean Peninsula and donated briquettes to the people at Kowloon Village in Gangnam-gu, Seoul.