In this study, an examination on the spectral, microstructural, and magnetic characteristics of Eu-Nd double-substituted Ba0.5Sr0.5Fe12O19 hexaferrites (Ba0.5Sr0.5NdxEuxFe12-2xO19 (x = 0.00-0.05) HFs) fabricated by an ultrasonic-assisted approach has been presented. An UZ SONOPULS HD 2070 ultrasonic homogenizer with frequency of 20 kHz and power of 70 W was used. The chemical bonding, structure and the morphology of the products were evaluated by Fourier-Transform Infrared (FT-IR) Spectroscopy, XRD (X-ray diffraction), scanning and transmission electron microscopy and techniques. The textural properties of the prepared nanomaterials were examined by using the Brunauer-Emmett-Teller (BET) method. The magnetic properties were studied using a vibrating sample magnetometer (VSM) at room temperature (RT) and low temperature 10 K. The magnitudes of various magnetic parameters including M-s (saturation magnetization), M-r (remanence) and H-c (coercivity) were estimated and evaluated. The M-H loops revealed the hard ferrimagnetic nature for all products at both temperatures. The M-s and M-r values showed a decreasing tendency with increasing degree of Eu3+ and Nd3+ substitutions whereas H-c values displayed an increasing trend. At RT, M-s, M-r and H-c values lie in the ranges of 63.0-68.8 emu.g(-1), 24.6-39.2 emu.g(-1) and 2252.4-2782.1 Oe, respectively. At 10K, the values of M-s, M-r and H-c lie between 87.5-97.1 emu.g(-1), 33.5-40.1 emu.g(-1) and 2060.6-2417.2 Oe, respectively. The observed magnetic properties make the prepared products promising candidates to be applied in the recording media.