In this paper, we examine the development of tailored 3D-structured (engineered) polymer-metal interfaces to create enhanced ionic polymer-metal composite (eIPMC) sensors towards soft, self-powered, high sensitivity strain sensor applications. First, a physics-based chemoelectromechanical model is developed to predict the sensor behavior of eIPMCs by incorporating structure microfeature effects in the mechanical response of the material. The model incorporates electrode surface properties, such as microscale feature thickness, size and spacing, to help define the mechanical response and transport characteristics of the polymer-electrode interface. Second, two novel approaches are described to create functional samples of eIPMC sensors using fused deposition manufacturing and inkjet printing technologies. Sample eIPMC sensors are fabricated for experimental characterization. Finally, experimental results are provided to show superior performance in the sensing capabilities compared to traditional sensors fabricated from sheet-form material. The results also validate important predictive aspects of the proposed minimal model.