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After the promotions of Brown Eyed Girls' fourth album, it was revealed that Gain had signed a contract with LOEN Entertainment to manage her solo career.
Prior to the release of her second EP, Gain was featured on Yoon Il-sang's anniversary album Yoon Il-sang 21st Anniversary Album: I'm 21 with a cover of "For You Not To Know" (Hangul: 너만은 모르길).
Gain herself became the second member to start her solo activities after Narsha by releasing her first mini-album, titled Step 2/4 with "Irreversible" as the title track in October, 2010, to critical acclaim from critics and public due to its strong influence of tango.
The video for the track was then released on October 8, 2010, alongside the album's release.
Beside from her activities with the group, she also had solo activities, beginning with her appearance in 4Tomorrow, a collaboration project with 4Minute's Hyuna, After School's UEE and KARA's Han Seung-yeon.
She also released a digital single, titled "We Fell in Love" (우리 사랑하게 됐어요) with then We Got Married partner 2AM Jo Kwon, composed by fellow member Je A, Kim Eana and produced by Lee Min-soo.
The collaborative EP debuted at number three on Gaon Albums Chart.
In April 13, 2013, she was featured in PSY's music video "Gentleman", along with the "arrogant" dance which was popularized in the Brown Eyed Girls song "Abracadabra".
Its title track, "Bloom", was also her best selling track and one of her signature hits to date.
At the beginning of 2014, Gain released her next EP, titled Truth or Dare, which featured lyrics from Kim Eana, Lee Hyo-ri and JYP, along with guest performers such as Bumkey and Jo Kwon, with the former being featured in the album's first single.
Considered as a "bolder" move for herself, the album was preceded by "Fxxk U", which received mixed reactions from the public due to its theme dealing with domestic violence; however, it was praised by critics.
The four members performed several small shows before officially debuting as Brown Eyed Girls in 2006.
In the same year, she performed a duet "Must Have Love" with SG Wannabe's leader Kim Yong Jun, which became her first number one hit during the Christmas season.