2D materials have been widely studied over the past decade for their potential applications in electronics and optoelectronics. In these materials, elemental composition plays a critical role in defining their physical properties. Here we report the first successful synthesis of individual high quality CuIn7Se11 (CIS) ternary 2D layers and demonstrate their potential use in photodetection applications. Photoconductivity measurements show an indirect bandgap of 1.1 eV for few-layered CIS, an external quantum efficiency of 88.0 % with 2 V bias across 2 μm channel with and a signal-to-noise ratio larger than 95 dB. By judicious choice of electrode materials, we demonstrate the possibility of layered CIS-based 2D photovoltaic devices. This study examines this ternary 2D layered system for the first time, demonstrating the clear potential for layered CIS in 2D material-based optoelectronic device applications.