In this study, the nonlinear optical properties of a new polymer poly crystal violet terephthalate (PCVT) as a solution and a thin film with different concentrations of 0.2, 0.6, and 1 mM and input power were investigated by using Z-scan technique at 532 nm CW laser beam wavelength. The negative nonlinear refractive index n2 as well as reverse saturable and saturable absorption β of the solution and film PCVT samples were determined. Figures of merit were also determined. In comparison with the Z-scan results, a self-diffraction pattern setup was used to measure nonlinear refractive index. Results showed a significant laser power dependence of the number of far-field diffraction rings with power and concentration, consistent with the Z-scan data. The PCVT sample exhibited good optical limiting behavior. Hence, PCVT has important nonlinear properties, and its figures of merit can be optimized by adjusting the PCVT concentration and input power. PCVT is a promising candidate for the design of optical photonic switching and optical limiter devices.