An ideal artificial bone will likely be multifunctional, combining different technologies to simultaneously promote bone regeneration while inhibiting microbial infection. In this study, copper- (Cu-) doped nano laponite (cnLAP) was prepared by a cation-exchanged method, and the cnLAP coating on poly(butylene succinate) (PBSu) scaffold was fabricated by poly(dopamine) modification. The results showed that incorporation of Cu ions into nano laponite (nLAP) did not have obvious effects on the morphology and surface area of cnLAP (compared with nLAP), which could be coated easily on macroporous PBSu scaffolds. In addition, the cnLAP-coated PBSu scaffolds could inhibit the growth of both Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus), indicating good antibacterial activity. Moreover, the cnLAP-coated PBSu scaffolds significantly promoted proliferation and improved alkaline phosphatase (ALP) activity of bone mesenchymal stem cells (BMSCs) compared with PBSu scaffolds. Furthermore, no obvious differences in cell responses to cnLAP- and nLAP-coated PBSu scaffolds were found, indicating that incorporation of Cu into nLAP had no negative effects on its cytocompatibility. The results suggested that the cnLAP-coated PBSu scaffolds exhibited excellent cytocompatibility and antimicrobial activity, which might offer promising opportunities for promoting bone regeneration and prevention of infectious from bacteria and effective treatment of bone defects.