Ultra-high-pressure jet processing (UHPJ) is a new non-thermal processing technique that can be employed for the homogenization and the sterilization of dairy products. However, the effects on dairy products are unknown when using UHPJ for homogenization and sterilization. Thus, this study aimed to investigate the effects of UHPJ on the sensory and curdling properties of skimmed milk and the casein structure in skimmed milk. Skimmed bovine milk was treated with UHPJ using different pressures (100, 150, 200, 250, 300 MPa) and casein was extracted by isoelectric precipitation. Subsequently, the average particle size, Zeta potential, contents of free sulfhydryl and disulfide bonds, secondary structure, and surface micromorphology were all used as evaluation indicators to explore the effects of UHPJ on the structure of casein. The results showed that with an increase of pressure, the free sulfhydryl group content changed irregularly, while the disulfide bond content increased from 1.085 to 3.0944 μmol/g. The content of α-helix and random coil in the casein decreased, while the β-sheet content increased at 100, 150, 200 MPa pressure. However, treatment with higher pressures of 250 and 300 MPa had the opposite effect. The average particle size of the casein micelles first decreased to 167.47 nm and then increased up to 174.63 nm; the absolute value of Zeta potential decreased from 28.33 to 23.77 mV. Scanning electron microscopy analysis revealed that the casein micelles had fractured into flat, loose, porous structures under pressure instead of into large clusters. After being ultra-high-pressure jet-processed, the sensory properties of skimmed milk and its fermented curd were analyzed concurrently. The results demonstrated that UHPJ could alter the viscosity and color of skimmed milk, shortening curdling time from 4.5 h to 2.67 h, and that the texture of the curd fermented with this skimmed milk could be improved to varying degrees by changing the structure of casein. Thus, UHPJ has a promising application in the manufacture of fermented milk due to its ability to enhance the curdling efficiency of skimmed milk and improve the texture of fermented milk.