With the global ageing population, the demand for innovative healthcare solutions for rehabilitating motor disabilities among the elderly is on the rise. Traditional healthcare facility-based rehabilitation is costly and time-consuming, limiting access to electrostimulation therapy for over 50% of the 2.4 thousand million potential beneficiaries. Dry electrodes, designed for extended use on sensitive skin, offer promise for monitoring surface electromyography and supporting muscular rehabilitation at home. These electrodes, which do not require conductive gels, improve patient comfort and reduce skin irritation in long-term biopotential recordings. Nevertheless, low impedance, stable electrochemical noise, flexibility, and biocompatibility are mandatory requirements for these electrodes. In this study, titanium–gold (Ti-Au) thin films were deposited on silicon and glass substrates using magnetron sputtering, and Glancing Angle Deposition (GLAD) was used to fully characterize them. The films were produced with gold compositions varying from 0 at.% to 44 at.%, growing in different geometries—conventional, inclined, and zigzag—using deposition angles ranging from 0° to 90°. The films' microstructure revealed a noticeable influence on the electrical properties of Ti-Au thin films, with electrical resistivity increasing by an order of magnitude at a deposition angle of 80° relative to the films prepared at 0° (conventional geometry). For the same deposition angle, no significant differences in electrical properties were observed between the inclined and zigzag geometries. This study intends to evaluate the influence of the chemical composition and the films’ growth geometry in terms of electrical properties, supporting the development of flexible Ti-Au thin film-based dry electrodes.