In this project, we fabricated electrospun nanofiber mats from pristine kafirin, the storage protein of sorghum, for the first time which have the potential to be used as eco-friendly food packaging materials. The first novel step was kafirin extraction which showed that the purity of kafirin was higher in double-purification compared to single-purification, which led to high quality nanosized round, straight, unbroken and unentangled fibers. The electrospinning results indicate that binary solvent, 75% (v/v) acetic acid (AcOH) and 25% (v/v) butanol (BuOH) mixture, allows fabrication of homogenous nanofiber mats at 0.4 g/ml kafirin-to-solvent ratio, which is critical for to obtain good mechanical strength for the mats. Encapsulation of thymol and carvacrol was successful when the loading concentrations were 0.1 g/ml and 0.1–0.2 g/ml, for thymol and carvacrol, respectively. Loading of the fibers with the bioactives was confirmed with FTIR where the characteristic peaks for the bioactives appeared at 950 cm−1, 1150 cm−1, 1200 cm−1 and 1250 cm−1. Thymol or carvacrol encapsulation led to the conversion of some of the β-turn structures of kafirin into β-sheet structures. Surface hydrophilicity of loaded kafirin fiber mats decreased with increasing carvacrol concentration and increased with increasing thymol concentration.