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The influence of Bi on the structure and physical properties of Ge2Se3-based equichalcogenide glasses and thin films is studied. Thermal analysis shows increased crystallization ability for Bi-modified glasses. Direct current (DC) and alternating current (AC) electrical conductivity for bulk glasses and thin films is investigated in a broad range of temperatures and frequencies, showing a strong dependence on the presence of Bi modifiers. Exposure wavelength dependence of photocurrent is studied at different temperatures for the visible range of spectrum, and correlated with the existence of localized states in the mobility gap of these amorphous semiconductors. Structural peculiarities of the obtained thin films and bulk samples are assessed from X-ray diffraction (XRD) and high-resolution X-ray photoelectron spectroscopy (XPS) measurements. Optical, electrical, and thermal properties are shown to be suitable for various applications in photonics, electronics, and sensor systems.