In this research, structural, magnetic, electrical, and optical properties of Al3+ substituted Ba0.6Sr0.4Ti1-xAlxO3 ceramics (where x = 0.00 to 0.20) have been investigated and discussed. The ceramic samples have been successfully synthesized by the conventional solid-state reaction method. The crystallinity of the prepared samples has been confirmed by X-ray peak broadening techniques such as the Williamson Hall (W-H) plot technique and the Scherrer method. The lattice constant "a", showing a significant drop as Al concentration increases, varies from 3.9420A to 3.9210A. The FTIR spectrum revealed a prominent peak between 435 cm−1 to 540 cm−1, without showing any secondary phase. Raman spectroscopic analysis showed that the prepared samples are in cubic phase with no phase transition. The shifting of a dominating peak in Raman at 580 cm-1 is due to the development of AlTi defects. VSM analysis at room temperature showed the ferromagnetic characteristics of all the samples. The highest value of the anisotropic constant (Ka~39.933 emu/cm3) has been seen at x=0.10. The real component of initial permeability is almost constant for the frequency range of about 75 MHz, and above this frequency range, it quickly reduces. At the high-frequency range, the prepared samples show an excellent relative quality factor due to the low dielectric loss, notably when x = 0.05. The prepared perovskites exhibited minimum eddy current loss characteristics due to the increment of AC resistivity at x=0.20. UV–visible spectroscopy shows a significant change in the energy bandgap from 3.23 eV to 3.04 eV with the doping concentrations.