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Current strategies for skeletal regeneration involve the use of autogenous and allogenic bone grafts that may not always be available or safe to use. One alternative is to develop materials for use as scaffolds for the tissue engineering of bone. We created architecturally nanofibrous scaffolds using the electrospinning technique. These calcium phosphate- based materials are porous, have a large surface-area-to-volume ratio and can be used to deliver drugs, biologics or cells for tissue engineering applications. Bone-matrix proteins were also conjugated to the surface of a polymer network of polycaprolactone and poly(2-hydroxyethyl methacrylate) to create a material with enhanced cellular responses. This biomimetic strategy resulted in favourable cell-surface interactions that will likely enhance bone-matrix synthesis and regeneration. These collective advancements enable the development of innovative scaffolds for applications in tissue engineering and bone regeneration.