Using an anionic surfactant, sodium dodecylbenzene sulfonate (SDBS), and a silane coupling agent, γ-aminopropyltriethoxysilane (KH550), as modifiers, 4A zeolite was modified to prepare two types of modified 4A zeolites (zeolite-SDBS and zeolite-KH550). Subsequently, poly(butylene adipate-co-terephthalate) (PBAT) was used as the matrix to prepare PBAT/modified 4A zeolite composite films via the solution casting method. The structures and properties of the two modified 4A zeolites were analyzed using FTIR, particle size, Zeta potential, and TGA tests. The effects of the content of the two modified 4A zeolites (based on the mass of PBAT) on the mechanical properties, thermal properties, water vapor permeability, and hydrophilicity of the PBAT/modified 4A zeolite composite films were investigated through tensile tests, TGA and DSC tests, water vapor transmission rate, and water contact angle measurements.The results indicated that, compared to 4A zeolite (median particle size 4.7 μm, Zeta potential 23.6 mV), the median particle sizes of zeolite-KH550 and zeolite-SDBS decreased (4.4 and 4.6 μm, respectively), and the surface negative charge increased (Zeta potential -46.2 and -45.8 mV, respectively). Compared to PBAT/4A zeolite composite films, the tensile strength, elongation at break, and initial decomposition temperature of PBAT/modified 4A zeolite composite films were improved. When the content of zeolite-KH550 and zeolite-SDBS was 20%, the tensile strength of PBAT/modified 4A zeolite composite films (15.4 and 13.5 MPa) increased by 22.2% and 7.1%, respectively, compared to PBAT/4A zeolite composite films (12.6 MPa). When the content of zeolite-KH550 and zeolite-SDBS was 30%, the elongation at break of PBAT/modified 4A zeolite composite films (331% and 303%) increased by 24.4% and 13.9%, respectively, compared to PBAT/4A zeolite composite films (266%). When the content of zeolite-KH550 and zeolite-SDBS was 40%, the initial decomposition temperature of PBAT/modified 4A zeolite composite films (370.9 and 370.7 ℃) increased by 1.3% compared to PBAT/4A zeolite composite films (366.1 ℃). Zeolite-SDBS was more conducive to inducing crystal nucleation but hindered crystal growth; the crystallization temperature of PBAT/modified 4A zeolite composite films prepared with zeolite-KH550 was relatively lower, but the crystallinity was relatively higher. Compared to zeolite-SDBS, PBAT/modified 4A zeolite composite films prepared with zeolite-KH550 exhibited better mechanical properties, thermal degradation performance, and water vapor barrier properties.