Nakajima's next single "Melody" was released on November 24, 2010; the songs included in the single were used in the original video animation Tamayura. She then performed the song "If", which was used as an insert song in the anime series Moshidora. This was followed by the release of the single "Kamisama no Itazura" (神様のいたずら) on October 26, 2011; the title song is used as the ending theme to the anime series Tamayura: Hitotose. Her next single, "Try Unite!/Hello!" was released on February 2, 2012; "Try Unite" was used as the opening theme to the anime series Lagrange: The Flower of Rin-ne. Her second album Be With You went on sale on March 3, 2012.
Nakajima's first non-Macross role was Miku in the anime series Akikan!. After that, she was cast as the character Citron in the series Basquash!; she along with Haruka Tomatsu and Saori Hayami performed the series' theme songs under the name Eclipse. She then played the role of Kaede Sakura in Kämpfer, and the roles of Chiho and Chise Mihara in Kobato. At the end of 2009, she voiced Ranka in the first movie of the Macross Frontier series, Macross Frontier the Movie: The False Songstress. In 2010, she played Lyra, a celestial spirit that belongs to Lucy Heartfilia, in the Fairy Tail series, and the character Lyra in Pokémon Diamond and Pearl. In February 2011, she voiced Ranka in the second Macross Frontier movie, Macross Frontier the Movie: The Wings of Goodbye. In 2012, she played the role of Meloetta in the anime theatrical short Meloetta's Moonlight Serenade, later reprising the role in the Pokémon: Black & White television series. She then voiced Yuzuki Eba in the original video animation A Town Where You Live, reprising the role the following year for the anime television series. In 2013, she played the role of Yō Kasukabe in Problem Children Are Coming from Another World, Aren't They?.