Multiple-color-emissive graphene quantum dots (GQDs) have great potential in diverse applications such as bioimaging, light emission, and photocatalysis. Growing interest in GQDs is largely focused on their macro-scale aggregations that could inherit the unique properties of individual dots. However, the lack of advanced fabrication methods limits the practical applications of GQDs. Here, we employed a Langmuir-Blodgett (LB) technique to fabricate ultrathin, high-quality GQD aggregated films with well-modulated optical properties in a wide range of wavelengths. Through the combination of a bottom-up synthesis of GQDs and the LB assembly method, uniform, closely packed, and ultra-thin GQD films can be self-assembled with a well-controlled thickness on different substrates. The photoluminescence (PL) spectra of ultra-thin GQD films have an obvious red-shift compared with isolated GQD solution. We then elucidate remarkably strong energy transfer in self-assembled GQDs. Furthermore, the ultra-thin GQD films exhibit a clear excitation-dependent PL that could almost cover the entire visible light. This convenient self-assembly method and systematic optical and physical studies of ultra-thin GQD films may provide a new direction for developing low-cost, GQD film-based light-emitting devices.