Engineering mussel-inspired multifunctional nanocomposite hydrogels to orchestrate osteoimmune microenvironment and promote bone healing

•A mussel-inspired strategy was proposed to fabricate bioactive hybrid hydrogels for bone regeneration.•The resulting hybrid hydrogel presented multifunction of osteogenic, angiogenic, and antibacterial activities.•Biohybrid hydrogels with favorable immunomodulation promoted osteogenesis via modulating macrophage M2 polarization.•The well-designed hydrogels possessed excellent therapeutic functions for immunomodulation and bone repair in vivo.