The high-power broadband terahertz (THz) generator is an essential tool for a wide range of THz applications. Here, we present a novel highly efficient electro-optic quinolinium single crystal for THz wave generation. For obtaining intense and broadband THz waves by optical-to-THz frequency conversion, a quinolinium crystal was developed to fulfill all the requirements, which are in general extremely difficult to maintain simultaneously in a single medium, such as a large macroscopic electro-optic response and excellent crystal characteristics including a large crystal size with desired facets, good environmental stability, high optical quality, wide transparency range, and controllable crystal thickness. Compared to the benchmark inorganic and organic crystals, the new quinolinium crystal possesses excellent crystal properties and THz generation characteristics with broader THz spectral coverage and higher THz conversion efficiency at the technologically important pump wavelength of 800 nm. Therefore, the quinolinium crystal offers great potential for efficient and gap-free broadband THz wave generation.