In this study, rubidium (Rb), cesium (Cs), and sodium (Na) alkali materials doped into CTS (Cu2SnS3), which is frequently used in semiconductor technology, were prepared to synthesize via ball milling method. CTS and Rb-, Cs, and Na-doped target crystal structures were recorded via XRD, and the surface images were monitored by SEM. Used raw solid powder materials were purchased and prepared to form targets in a laboratory environment, and the generated targets were placed in glass vessel to produce nanoparticles in ethanol using femtosecond laser ablation technique. In the SEM images of CTS, it was seen that the average nanoparticle size in the liquid was around 57 nm. The produced nanoparticles in liquid were analyzed with linear optical properties by UV-Vis absorption spectroscopy and nonlinear optical properties with z-scan technique. Numerical values of nonlinear absorption coefficients, refractive index, and third-order susceptibility were calculated and given to be in the order of 10−16 W/cm2, 10−10 W/cm, and 10−13 esu ratios, respectively. The study also includes important results on the use of the results obtained in nonlinear photonic technology.