Cellulose acetate (CA)/strontium phosphate (SrP) hybrid coating has been proposed as an effective strategy to build up novel bone-like structures for bone healing since CA is soluble in most organic solvents. Strontium (Sr2+) has been reported as a potential agent to treat degenerative bone diseases due to its osteopromotive and antibacterial effects. Herein, bioactive hybrid composite SrP-based coatings (CASrP) were successfully produced for the first time. CASrP was synthesized via a modified biomimetic method (for 7—CA7dSrP, and 14 days—CA14dSrP), in which the metal ion Sr2+ was used in place of Ca2+ in the simulated body fluid. Energy-dispersive X-ray (EDX) and Fourier transform infrared spectroscopy (FTIR) analysis confirmed the SrP incorporation chemically in the CASrP samples. Atomic absorption spectroscopy (AAS) supported EDX data, showing Sr2+ adsorption into CA, and its significant increase with the augmentation of time of treatment (ca. 92%—CA7dSrP and 96%—CA14dSrP). An increment in coating porosity and the formation of SrP crystals were evidenced by scanning electron microscopy (SEM) images. X-ray diffraction (XRD) evidenced a greater crystallinity than CA membranes and a destabilization of CA14dSrP structure compared to CA7dSrP. The composites were extremely biocompatible for fibroblast and osteoblast cells. Cell viability (%) was higher either for CA7dSrP (48 h: ca. 92% and 115%) and CA14dSrP (48 h: ca. 88% and 107%) compared to CA (48 h: ca. 70% and 51%) due to SrP formation and Sr2+ presence in its optimal dose in the culture media (4.6–9 mg·L−1). In conclusion, the findings elucidated here evidence the remarkable potential of CA7dSrP and CA14dSrP as bioactive coatings on the development of implant devices for inducing bone regeneration.