<p>High-performance and cost-effective, soft magnetic composites (SMCs) are strategic materials for the miniaturization of microelectronic devices. Outmoded SMCs incorporate thicker insulating layers at particle surfaces to reduce eddy current loss at KHz and MHz frequencies, which affects their magnetic induction density and compromises magnetic performance and mechanical strength. In this paper, acetic acid-modified TiO₂ nanoparticles (NPs) are consistently deposited on the surface of FeSiCr alloy particles by electrostatic deposition, resulting in a nano-sized insulated TiO₂ layer on the surface of FeSiCr via a wet chemical process. The as-formed TiO₂ NPs layers on FeSiCr alloy particles effectively reduce power loss at kHz and MHz frequencies, endowing the material with high-frequency stability, excellent mechanical strength, and enhanced effective permeability. At the KHz frequency range, FeSiCr-0.1wt%TiO₂ SMC exhibits a low power loss of 165 kW m⁻³ (50mT/50 kHz) and a high effective permeability of 87. At the MHz frequency range, the FeSiCr-0.2wt%TiO₂ SMC exhibits a low power loss of 275.34 kW m⁻³ (5mT/10MHz), which is 78% lower than other reports, the real part of complex permeability 74, stable till 40 MHz, and a cutoff frequency as high as 170 MHz. In addition, these SMCs withstand high DC bias more than 73% for all percentages of coating materials. Additionally, we employed first-principles simulations to investigate the electronic structure and mechanical properties of the FeSiCr/TiO₂ composite. Computational studies demonstrate charge transfer at the FeSiCr/TiO₂ interface, facilitating strong covalent bonding between the constituent layers. A favorable formation energy stabilizes the resulting interfacial structure. This study provides an efficient route for forming high-performance SMC, which is both economical and offers higher permeability values at KHz–MHz frequencies, suitable for application in soft magnetic devices.</p>