In this study, an enhanced methodology for the synthesis and crystallization of Voclosporin was devised. Isopropyl acetate was selected as the solvent for the acetylation reaction, resulting in a substantial reduction in the reaction duration from 4 days to 15 h. The reagent (E)-trimethyl(3-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl)prop-1-en-1-yl)silane (8) was chosen for the Peterson reaction, achieving a conversion rate exceeding 90%. Subsequently, 1,8-diazabicyclo[5,4,0]undec-7-ene (DBU) was employed as the hydrolysis reagent for deacetylation, yielding an E/Z ratio of 97:3. Moreover, the use of an ethanol/water mixture as the crystallization solvent facilitated the production of Voclosporin in its crystalline form, obviating the need for column separation and purification steps. In summary, a successful four-step process for producing Voclosporin was achieved, yielding a 50% overall yield with a high-performance liquid chromatography purity of 98.8%. The crystal form of Voclosporin was investigated, resulting in the acquisition of a sizable crystal, and the crystallographic structure of Voclosporin was documented. Our data hold significant value for advancing the understanding of both the synthetic methodology and the crystal stability of Voclosporin.