Pediococcus acidilactici was used to ferment fresh pork. After fermentation, the pork jerky was subjected to sensory evaluation and the levels of pH, free amino acids, and volatile compounds were measured. The results showed that the fermented pork jerky had a better sensory evaluation score (score: 93.2), lower pH value (3.54), and more free amino acids (39.24 mg/100 g). Furthermore, in the fermented pork jerky, the content of three acids (18.552%) was high, which lowered the pH of the pork jerky and inhibited growth of pathogens. Moreover, some new compounds produced, including 3-hydroxy-2-butanone (49.095%), 2,3-butanediol (2.790%), 2-ethyl-1-hexanol (2.400%), oxalic acid isobutyl hexyl ester (2.280%), phenylethyl alcohol (0.953%), and eucalyptol (0.659%), contributed to the flavour of pork jerky. Overall, our results demonstrated that P. acidilactici can be used for the production as well as improvement of the quality and flavour of fermented pork jerky.