Dual-modifications of jet milling and hydroxypropylation were used to improve the functional properties of maize starch (HM, containing 67 % amylose). The fractions obtained in three sizes (HM-S, HM-M, HM-L) were further treated with 10 % and 30 % propylene oxide (PO10 and PO30). The infrared peak of starch at 2794 cm−1 indicated the successful introduction of hydroxypropyl groups. The molar degree of substitution (MS) increased with the degree of jet milling. The MS of HM-L-PO10 is 0.4, that of HM-M-PO10 is 0.7, and that of HM-S-PO10 is 0.9. The crystallinity of dual-modified HM increased, but the crystal type remained unchanged, still being B-type. Dual-modification significantly improved the performance of starch, and the higher the degree of modification, the better the optimization effect. The lowest enthalpy changes of gelatinization (ΔH = 3.49 J/g), the best freeze–thaw stability, the highest elongation at break (110.42 %) and transmittance (81.22 %) were shown in HM-S-PO30. The present study confirms that HM-S-PO30 films have the best physicochemical and mechanical properties, which provide new insights into optimizing starch-based packaging materials.