Recent advancements in materials synthesis and processing technology, coupled with a deeper understanding of bone nanoscale structure and biology, have provided new avenues for designing bioactive materials in bone tissue regenerative medicine. This Review focuses on the design and application of polydopamine-modified polycaprolactone scaffolds loading metal nanoparticles for bone tissue engineering. We explore their antibacterial properties and their ability to guide cell behavior. Specifically, we discuss the synthesis techniques, protein deposition, morphology variations, and interactions with the extracellular matrix of these scaffolds and biocompatibility and efficacy in promoting bone tissue regeneration in vitro and in vivo. Challenges and unmet needs are reviewed in the development of polymer- and metal-based materials for bone tissue engineering.