Silver nanoparticles have quickly established themselves as a multifaceted nanomaterial in the biomedical field, with their properties widely studied over the last decade. However, there are still concerns regarding its long-term toxicity. Recent developments in nanoparticle fabrication and surface manipulation using various biomolecules have enabled the preparation of nontoxic nanosilver. Thus, nanosilver has been safely incorporated into a variety of regenerative templates for the engineering of tissues such as the cornea, skin, and heart. In addition, it has been incorporated into wound-healing treatments, biosensors, and imaging modalities, among others. In this chapter, a selection of promising synthetic routes for the preparation of biomolecule-capped silver nanoparticles will be discussed and presented. The main goal is to present a rationale for choosing a synthetic route for nanosilver that minimizes/avoids toxic side effects for biomaterial development.