To overcome the limitations associated with the high volatility, pungent odor, and restricted application of α-terpineol in food packaging, α-terpineol-loaded microcapsules were prepared using the ionic gelation method, with α-terpineol as the core material and chitosan (CS) as the wall material. Based on single-factor experiments, the preparation process was further optimized using response surface methodology. The results demonstrated that the mass ratio of CS to α-terpineol, the mass ratio of CS to sodium tripolyphosphate (TPP), and the pH of the chitosan solution significantly affected the encapsulation efficiency, with the degree of influence ranked as follows: CS: α-terpineol > CS: TPP > pH. The optimal preparation conditions were determined as follows: CS: α-terpineol ratio of 1:0.75, CS:TPP ratio of 2.2:1, and pH 4.9, under which the encapsulation efficiency reached 73.85%. Under these optimized conditions, the microcapsules exhibited superior sustained-release behavior in phosphate buffer solution (pH 7.4), with a cumulative release rate of only 35.8% after 312 h. The developed microencapsulation system effectively retarded the diffusion rate of α-terpineol, providing an important basis for its broader application in food packaging systems.