Transition metal dichalcogenides (TMDs) have provided a fundamental stage to study light–matter interactions and optical applications at the atomic scale due to their ultrathin thickness and their appropriate band gap in the visible region. Here, we report the strong nonlinear optical effects, including second-harmonic generation (SHG) and third-harmonic generation (THG) in spiral WS2 structures. SHG intensity quadratically increases with layer numbers, other than diminishing the oscillation of 2H stacking TMDs. The contrary SHG behavior is attributed to the broken symmetry from twisted screw structures, revealed by aberration-corrected transmission electronic microscope observation. Furthermore, the twist angle of the screw structure (5 degrees) was obtained by high-resolution transmission microscope measurements and confirmed by polarization tests of SHG output. Moreover, we roughly estimate the effective second-order nonlinear susceptibility. The discovery and understanding of the accumulation of nonlinear susceptibility of spiral structures with increasing thickness will extend the nonlinear applications of TMDs.