Recently, quasi-complementary sequence sets (QCSSs) including low correlation zone complementary sequence sets (LCZ-CSSs), and low correlation complementary sequence sets (LC-CSSs) have raised lots of concerns. According to the theoretical bounds, the set size of a QCSS is much larger than that of a traditional perfect complementary sequence set (PCSS). As a result, it is believed that QCSSs have potential applications in multi-carrier code-division multiple-access (MC-CDMA) systems to support more users. As binary sequences are desired in practice because of easier realization, we consider the design of binary QCSSs with large set size in this letter. A construction of aperiodic binary LCZ-CSSs is proposed, which leads to aperiodic binary LCZ-CSSs with asymptotically optimal parameters. Additional, aperiodic binary LC-CSSs with asymptotically optimal parameters can also be derived from the proposed construction.