Aiming at biosignal acquisition for bioelectrodes application, Ti–Ag thin films were produced by GLAD, in order to tailor their electromechanical properties. The electrical behavior of the sculptured Ti–Ag thin films was studied with increasing annealing temperatures. The results revealed a good correlation with the set of morphological features displayed. With the increase of the vapor flux angle, a more defined structure was obtained, as well as a more porous morphology, which increased the electrical resistivity of the coatings. An important point consists in the recrystallization of Ti–Ag intermetallic phases due to the temperature increase (between 558 K and 773 K), which resulted in a sharp decrease of the electrical resistivity values.