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A wide variety of composite scaffolds with unique geometry, porosity and pore size can be fabricated with versatile 3D printing techniques. In this work, we fabricated 3D-printed composite scaffolds of polycaprolactone (PCL) incorporating bioactive glass (BG) particles (13-93 and 13-93B3 compositions) by using fused deposition modeling (FDM). The scaffolds were modified with a “mussel-inspired surface coating” to regulate biological properties. The chemical and surface properties of scaffolds were analyzed by Fourier transform infrared spectroscopy (FTIR), contact angle and scanning electron microscopy (SEM). Polydopamine (PDA) surface-modified composite scaffolds exhibited attractive properties. Firstly, after the surface modification, the adhesion of a composite coating based on gelatin incorporated with strontium-doped mesoporous bioactive glass (Sr-MBGNs/gelatin) was significantly improved. In addition, cell attachment and differentiation were promoted, and the antibacterial properties of the scaffolds were increased. Moreover, the bioactivity of these scaffolds was also significantly influenced: a hydroxyapatite layer formed on the scaffold surface after 3 days of immersion in SBF. Our results suggest that the promoting effect of PDA coating on PCL-BG scaffolds leads to improved scaffolds for bone tissue engineering.