We describe an innovative and simple drop-cast processing strategy to create bonelike multicomponent bionanocomposite materials that consist of an organic poly(ε-caprolactone) (PCL) matrix, minerals such as hydroxyapatite (HAP) and CaCO3, and collagen fibers. The process allows morphological and structural control to achieve the desired nanostructure of the bone mimics. The fabrication method involves adding inorganic and organic components sequentially followed by controlling the growth conditions and composition. This enables organization of collagen nanofibers (∼ 100 nm) into scaffolds while simultaneously allowing nucleation and co-alignment of hydroxyapatite spheres (∼ 100 – 500 nm) within aligned, thermally stable collagen fibers in the porous PCL matrix. We achieved high calcium (26%) and oxygen (17%) within the bioscaffold and adequate phosphorous compositions comparable to the levels of bone tissues. Adequate mineralization along with high oxygen content may help maintain the required bone mineral density and revascularization for nutrient and compensate for the loss of oxygen delivered to the bone cells. Furthermore, since the bionanocomposite scaffold is made of natural materials (calcium, phosphorous and collagen) found in bone tissue, the formulation makes it an excellent biocompatible/biodegradable material. Our preliminary results suggest huge potential of these advanced bionanocomposite scaffolds for bone substitutes and tissue engineering applications.