In this work, soluble soybean polysaccharides (SSPS) were employed together with multifrequency ultrasound to fabricate zein nanocomposites which were conducive to enhancing the stability of high internal phase emulsions (HIPEs). Compared with non-ultrasonic treated zein colloidal particle samples (132.23 ± 0.85 nm), the zein nanoparticles samples induced by dual-frequency ultrasound exhibited a smaller particle size (114.54 ± 0.23 nm). Furthermore, the particle size of the zein composite nanoparticles (256.5 ± 4.81) remarkably increased with SPSS coating, consequently leading to larger fluorescence intensity together with lower zeta-potential (-21.90 ± 0.46 mv) and surface hydrophobicity (4992.15 ± 37.28). Meanwhile, zein-SSPS composite nanoparticles induced by DFU showed remarkably enhanced thermal stability. Fourier transform infrared (FTIR) spectroscopy and Circular dichroism (CD) spectroscopy were also used to characterize zein-SSPS composite nanoparticles. The results confirmed that DFU combined with SSPS treatment significantly increased β-sheets (from 12.60% ± 0.25 b to 21.53% ± 0.37 c) and reduced α-helix content (34.83% ± 0.71 b to 23.86% ± 0.66 a) remarkably. Notably, HIPEs prepared from zein-SSPS nanocomposites induced by dual-frequency simultaneous ultrasound (DFU) at 40/60 kHz showed better storage stability. HIPEs stabilized by DFU induced zein-SSPS nanoparticles exhibited higher storage modulus (G') and loss modulus (G″), leading to lower fluidity, together with better stability contributing to the water-binding capacity and three-dimensional (3D) network structure of the HIPEs emulsion. The findings of this study indicate that this method can be utilized and integrated to further extend the application of zein and SSPS and explore HIPEs.