摘要： Structurally chiral materials hosting multifold fermions with large topological number have attracted considerable attention because of their naturally long surface Fermi arcs and bulk quantized circular photogalvanic effect (CPGE). Multifold fermions only appear in metallic states, and therefore most studies so far have only focused on the semimetals in compounds with chiral crystal structures. In this work, we show that the structurally chiral topological trivial insulators are also exotic states, which is interesting from the application point of view, owing to their natural advantage to host a large bulk photovoltaic effect in the visible wavelength region. In recent decades, the shift current in the visible wavelength region was limited to be 10 μA/V2 in all the experimentally measured reports. By scanning the insulators with chiral structure, we found a class of compounds with photoconductivity ranging from ～20 to ～80 μA/V2, which is comparable to the largest reported shift current. This work illustrates that the compounds with chiral structure can host both quantum CPGE and a strong shift current in the second-order optical response. Moreover, this work offers a good platform for the study of the shift current and its future application by putting the focus on insulators with chiral lattices, so far overlooked in photovoltaic technologies.