We demonstrate the deliberate activation or inhibition of invitro angiogenesis using functional peptide coated gold nanoparticles. The peptides, anchored to oligo-ethylene glycol capped gold nanospheres, were designed to selectively interact with cell receptors responsible for activation or inhibition of angiogenesis. The functional particles are shown to influence significantly the extent and morphology of vascular structures, without causing toxicity. Mechanistic studies show that the nanoparticles have the ability to alter the balance between naturally secreted pro- and anti-angiogenic factors, under various biological conditions. Nanoparticle-induced control over angiogenesis opens up new directions in targeted drug delivery and therapy.