The objective of this work is to investigate the chemical and nutritional value of milk thistle meal (MTM) in order to improve it and to provide theoretical support for its application in dairy cattle production. MTM was assessed in comparison with seven conventional protein feed sources, namely, soybean meal (SBM), cottonseed meal (CS), canola meal (CN), palm kernel meal (PK), rice bran meal (RB), corn germ meal (CG), and sesame meal (SS). The chemical composition of these feedstuffs was assessed using wet chemical analysis, the Cornell Net Carbohydrate and Protein System was used to evaluate the carbohydrate and protein fractions, and the in situ nylon bag technique and the modified three-step in vitro method were used to assess the rumen degradation and intestinal digestibility. Additionally, Fourier transform infrared technology was used to determine the feedstuff protein spectral molecular structure and its amino acid profile was also assessed. The result showed that MTM acid detergent fiber, lignin, unavailable nitrogen, and non-degradable carbohydrate content were higher than those of the other feedstuffs. It had a 17% and 36% rumen effective degradation rate of neutral detergent fiber and dry matter, respectively, and had the lowest small intestinal rumen undegradable protein digestibility rate. It was low in leucine, histidine, arginine, and proline, but high in methionine. The total area of amide I and amide II in the protein secondary structure was similar to that of CN and CS, and the amide I and II ratio was not different from that of RB. To sum up, MTM has a poor carbohydrate composition and is high in fiber but, in comparison to most other protein feeds, has a higher crude protein rumen effective degradation rate, similar to that of SBM, and it is a good source of methionine, a limiting amino acid. Hence, its nutritional value can be further improved for application in dairy feeding through processes such as microbial or enzymatic fermentation.