Soy protein-based films often exhibit poor properties, including limited mechanical strength, stability, and bioactivity, which hinder their extensive application in the food industry, particularly in edible packaging. To enhance the properties of soy protein-based films, we employed high-pressure homogenization (HPH) to modify the soybean protein isolate (SPI) molecules and sought to cross-link SPI with ulvan polysaccharide, which possesses distinctive bioactivities. The results confirmed that soluble ulvan polysaccharides were incorporated into the cross-linking system through hydrogen bonding. Results indicated that HPH treatment enhanced SPI's solubility and surface hydrophobicity (H0), promoting hydrogen bonding and hydrophobic interactions between SPI and ulvan, as evidenced by ζ-potential and turbidity measurements. Structural and microstructural analyses of both individual SPI and composite films, using FT-IR, XRD, CD and SEM, demonstrated a high compatibility between HPH-treated SPI and ulvan. The incorporation of ulvan reduced the films' tensile strength (TS), but higher pressure significantly improved it (p < 0.05). Post-HPH modification, the films exhibited increased contact angle and swelling capacity (p < 0.05), indicating enhanced hydrophobicity. Higher pressure treatments resulted in more opaque and yellowish films, thereby diminishing ultraviolet light transmission. Thermal stability analyses, via TGA-DSC, showed that U-HSPI films had improved thermal stability compared to pure SPI films. Moreover, ulvan inclusion boosted the antioxidant capacity of SPI films, especially after HPH treatment. Overall, this study confirms that HPH modification substantially influences the properties and activities of SPI-based films, and the complex films based on SPI and ulvan with improved physicochemical and antioxidant properties exhibit a great potential in the food packaging field.