In this study, we report on the design, synthesis, and full characterization of a covalently-linked, triclosan silica-based nanoparticles (T-SNPs), coated with a polyaminated shell (NH2-T-SNPs). Various techniques are used to elucidate and rationalize the potential biological mechanism of action of these novel nanoparticles. NH2-T-SNPs are found to be potently bactericidal with no detectable lag time for the antimicrobial activity against E. coli and S. aureus. In this context, we also prove that triclosan is the chemical agent that mediated the bactericidal activity of these chemically-modified NPs. The obtained experimental data allows us to pinpoint the actual minimal bactericidal concentrations (MBCs) of triclosan-bound NPs by quantifying intracellular triclosan concentrations. Furthermore, we conduct preliminary cytotoxicity studies, which show that triclosan bound NPs are less cytotoxic (2000 fold) in vitro compared to free-triclosan when tested with various human and mammalian cell lines. Taken together, our results further support the characterization and development of these new nanoscale materials for various biomedical applications.