Bone repair and regeneration is a persistent clinical challenge, leading to numerous methods being attempted for treating defects. Still, the need to develop alternative repair strategies exists. Bone is a composite material consisting of two predominant matrix components, collagen type I and hydroxyapatite. Piezoelectric potential in bone is prompted by these organic and inorganic materials, allowing this tissue to convert applied mechanical stresses into electrical currents within itself. Due to natural tissue graft limitations, regenerative and tissue engineering strategies involving the combination of biocompatible synthetic scaffolds and osteogenic cells have emerged as a promising approach for repairing damaged bone. However, the synthetic materials typically used lack the necessary bioactive properties to participate fully in tissue regeneration. This dissertation explores the benefits of using stimuli-responsive or “smart” biomaterials as hard tissue replacements through a series of systematic and biomimetic scaffolding developments presented in sequential chapters. First, an overview of current bone tissue engineering challenges and the promising future that conductive materials present towards alleviating issues associated with bone repair and regeneration is given. The second chapter provides a study of the combined efficacy of 3D-printed conductive polymeric scaffolds with exogenous electrical stimulation (ES). Murine preosteoblasts exposed to ES on conductive scaffolding differentiated into mature osteoblasts considerably faster than on non-conductive scaffolds, substantiating the combined benefits of electroconductive materials and ES for bone formation. The third chapter describes the feasibility of producing printable biohybrid composite scaffolds capable of supporting electrical signaling with retained bioactivity. Human bone marrow-derived mesenchymal stromal cells (hMSCs) cultured on conductive composites and exposed to ES displayed earlier signs of osteoblastic differentiation compared to cells on conductive polymer-only control scaffolds, confirming the correlation between improved scaffold bioactivity and rapid osteogenesis. Lastly, a culminating study to assess the functionality of piezoelectric bioprinted bone scaffolds under dynamic culturing conditions (i.e., ultrasonic stimulation) is discussed. The prepared scaffolds displayed promising piezoelectric characteristics and provoked increased mineral deposition from seeded hMSCs. Altogether, using “smart” biomaterials as synthetic scaffolding for bone offers substantial benefit over currently used methods, and could potentially provide better surgical outcomes to improve high-risk reconstructive surgeries through additive manufacturing techniques.