Piezoresistive sensors composed of nickel nanostrands, nickel-coated carbon fibers, and silicone can be used to measure large physical deflections but exhibit viscoelastic properties and creep, leading to a complex and nonlinear electrical response that is difficult to interpret. This study considers the impact of modifying the geometry and architecture of the sensors on their mechanical and electrical performance. Varying the sensor thickness leads to potentially significant differences in conductive fiber alignment, while adding external layers of pure silicone provides elastic support for the sensors, potentially reducing their extreme viscoelastic nature. The impact of such modifications on both mechanical and electrical behavior was assessed by analyzing strain to failure, the magnitude of hysteresis with cycling, the repeatability of the electro-mechanical response, the strain level at which resistance begins to monotonically decrease, and the drift in electrical response with cycling. The results indicate that thicker single-layer sensors have less electrical drift. Sensors with a multilayered architecture exhibit several improvements in behavior, such as increasing the range of the monotonic region by approximately 52%. These improvements become more significant as the thickness of the pure silicone layers increases.