Tm-Tb co-substituted Co-Ni nanospinel ferrites (NSFs) as (Co0.5Ni0.5) [TmxTbxFe2−2x]O4 (x = 0.00–0.05) NSFs were attained via the ultrasound irradiation technique. The phase identification and morphologies of the NSFs were explored using X-rays diffraction (XRD), selected area electron diffraction (SAED), and transmission and scanning electronic microscopes (TEM and SEM). The magnetization measurements against the applied magnetic field (M-H) were made at 300 and 10 K with a vibrating sample magnetometer (VSM). The various prepared nanoparticles revealed a ferrimagnetic character at both 300 and 10 K. The saturation magnetization (Ms), the remanence (Mr), and magneton number (nB) were found to decrease upon the Tb-Tm substitution effect. On the other hand, the coercivity (Hc) was found to diminish with increasing x up to 0.03 and then begins to increase with further rising Tb-Tm content. The Hc values are in the range of 346.7–441.7 Oe at 300 K to 4044.4–5378.7 Oe at 10 K. The variations in magnetic parameters were described based on redistribution of cations, crystallites and/or grains size, canting effects, surface spins effects, super-exchange interaction strength, etc. The observed magnetic results indicated that the synthesized (Co0.5Ni0.5)[TmxTbxFe2−x]O4 NSFs could be considered as promising candidates to be used for room temperature magnetic applications and magnetic recording media.