Bone tissue has an anisotropic structure, which is strongly associated with the collagen fibril orientation and the direction of the c-axis of the bone apatite crystal. The bone regeneration process contains two main phases: bone mineral density (BMD; bone quantity) restoration and reconstruction of the bone apatite c-axis orientation (bone quality), which is the dominant factor for the mechanical properties of bone. Hence, restoration of the bone quality and quantity is required for bone tissue regeneration. In this work, novel, oriented siloxanecontaining vaterite/poly(lactic acid) composite scaffolds were developed by controlling the cell alignment and proliferation, which play an important role in regenerating the bone quality and quantity, respectively. Our strategy controlled the cell alignment and proliferation using a morphological design of the scaffolds and the ions released from the siloxanecontaining vaterite. The scaffolds were designed to control of the cell alignment, which successfully induced cell orientation along the fibermats. In addition, the released ions from the siloxane-containing vaterite improved osteoblast proliferation, indicating that the released Mg 2+ and silicate ions stimulated cell adhesion and proliferation. These results indicated that the fibermats developed in this work could be used for bone tissue regeneration scaffolds that enable the recovery of bone quality and quantity.