Strontium folate (SrFO) is a recently developed bone promoting agent with interest in medical and pharmaceutical fields due to its improved features in comparison to current strontium based therapies for osteoporosis and other bone diseases. In this work SrFO derivative was synthesized and loaded into biohybrid scaffolds obtained through lyophilisation of semi-interpenetrating networks of chitosan polyethylene glycol dimethacrylate and beta tri-calcium phosphate (βTCP) fabricated using free radical polymerization. The scaffolds were seeded with pluripotent stem cells obtained from human dental pulp and their potential to regenerate bone tissues were assessed using a critical sized defect model of calvaria in rats and compared with those obtained without SrFO. The results obtained both in vitro and in vivo demonstrated excellent cyto-compatibility with resorption of scaffolds in 4–6 weeks and a total regeneration of the defect, with a more rapid and dense bone formation in the group with SrFO. Thus, the use of stem cells sourced from human dental pulp in combination with SrFO are very promising systems for their application in compromised osseous tissue regeneration.