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The spinal surgeon community has expressed significant interest in applying calcium phosphate cement (CPC) for the treatment of vertebral compression fractures (VCFs) and minimizing its disadvantages, such as its water-induced collapsibility and poor mechanical properties, limiting its clinical use. In this work, novel biodegradable electrospun nanofibrous poly(d,l-lactic acid-ϵ-caprolactone) balloons (ENPBs) were prepared, and the separation, pressure, degradation, and new bone formation behaviors of the ENPBs when used as CPC-filled containers in vitro and in vivo were systematically analyzed and compared. CPC could be separated from surrounding bone tissues by ENPBs in vitro and in vivo. ENPB-CPCs (ENPBs serving as CPC-filled containers) exerted pressure on the surrounding bone microenvironment, which was enough to crush trabecular bone. Compared with the CPC implantation, ENPB-CPCs delayed the degradation of CPC (i.e., its water-induced collapsilibity). Finally, possible mechanisms behind the in vivo effects caused by ENPB-CPCs implanted into rabbit thighbones and pig vertebrae were proposed. This work suggests that ENPBs can be potentially applied as CPC-filled containers in vivo and provides an experimental basis for the clinical application of ENPBs for the treatment of VCFs. In addition, this work will be of benefit to the development of polymer-based medical implants in the future.