In this study, BaO–TiO2–SiO2 (BTS) glasses and glass–ceramics doped with ZrO2, having the composition (30 − x)BaO•30TiO2•40SiO2•x[ZrO2] (x = 0, 2, 4, and 6 mol%), were synthesized using the melt-quenching technique followed by sintering at 1000 °C for 4 h. Varying ZrO2 content led to improved physical properties, including an increase in both the green (un-sintered) density (from 3.08 to 3.55 g/cm3) and sintered density (from 3.87 to 4.28 g/cm3). X-ray diffraction (XRD) analysis verified that the fabricated glasses exhibited an amorphous structure. Moreover, XRD analysis of the synthesized glass ceramics (GCs) revealed that higher ZrO2 content and heat treatment facilitated the transition from an amorphous to a crystalline structure, with a dominance of primary phase of tetragonal Ba2TiSi2O8 along with secondary phase of monoclinic ZrO2. Furthermore, the fabricated GCs were characterized using FTIR spectroscopy, X-ray photoelectron spectroscopy (XPS), field emission scanning electron microscopy (FESEM), elemental mapping, a universal testing machine (UTM) for compression testing, hardness measurements, tribological evaluation, and impedance spectroscopy. FESEM analysis of all samples revealed a complex morphology with interconnected grains and a progressive reduction in residual glassy phases. Moreover, mechanical analysis showed significant improvements with rising ZrO2 content, with BTSZC6 (x = 6 mol% ZrO2) achieving a compressive strength of 604 MPa, fracture toughness of 41.59 MPa·m1/2, and hardness of 866.2 HV. Moreover, tribological results showed that BTSZC6 had the lowest wear volume of 0.13 mm3 (10 N), while BTSZC2 (x = 2 mol% ZrO2) recorded the lowest friction coefficient at 0.16 (10 N). Notably, the BTSZC6 sample exhibited an exceptional dielectric constant (⁓ 4704) with a low dielectric or tangent loss of about 0.09 at 10 Hz (500 °C), accredited to the space charge or interfacial polarization. These properties make the GCs promising candidates for the production of multilayer ceramic capacitors and electronics devices.