To investigate the mechanism of yeast inoculation on aroma improvement of Jinhua ham, microbial succession, myofibrillar protein hydrolysis, enzyme activities, amino acid metabolism, volatile compound evolutions, sensory attributes, and the relationship between key volatiles and sensory attributes were investigated during the processing of Jinhua ham with the inoculation of Rhodotorula mucilaginosa AUMC 9298 (RM), Candida parapsilosis d70a (CP) or Pichia kudriavzevii XS-5 (PK), respectively, while ham samples without any inoculation were defined as the control group (CK). The inoculation of RM, CP, and PK significantly increased the counts of fungal communities, and the fungal counts of the final products after dry-ripening for 40 days reached 6.65, 6.33, 7.35, and 7.55 (lg (CFU/g)) in CK, PK, RM, and CP groups, respectively; the treatment of RM showed the highest sensory scores in meaty aroma, nutty aroma, and overall acceptance among these groups. The treatment of RM showed the highest capability to degrade myosin and actin. The total contents of free amino acids increased significantly from 2 565.89 mg/100 g of PK to 3 141.46 mg/100 g of RM and 2 714.76 mg/100 g of CP in the final products (P < 0.05), and the most release of free amino acids was observed in RM among these groups. The activities of keto acid decarboxylase, aromatic and branched chain aminotransferase, and branched chain amino acid dehydrogenase in RM were significantly higher than those of CP and PK, which contributed to the metabolism of aromatic and branched chain amino acids. Gas chromatography-mass spectrometry and multivariate statistics demonstrated that benzaldehyde, 3-methylbutanal, 2,5-dimethylpyrazine, and 2,6-dimethylpyrazine were responsible for the improvement of overall acceptance of Jinhua ham with RM inoculation.