We have presented a non-covalently cross-linked hybrid nano- composite, which outperforms conventional, covalently cross- linked analogs in terms of self-healing capacity as well as adhe- siveness to mineral surfaces. Most importantly, these non- covalently cross-linked composites were surprisingly robust yet biodegradable upon extensive in vitro and in vivo testing, thereby confirming that cohesive nanocomposites can be developed based on reversible bonds between polymer-grafted bisphosphonate li- gands and calcium ions as present on the surface of nanoscale inorganic particles. The biological observation that a hydrogel based on such reversible bonds aids in the progression of bone formation throughout the material is particularly appealing for bone regenerative applications.