N-Aminoimidazolidin-2-one (Aid)-containing peptides with a constrained backbone present a novel class of peptidomimetics for drug discovery. The introduction of Aid residues into peptide sequences has been achieved by intramolecular Mitsunobu cyclization of a serine side chain onto the α-NH of an aza-glycine residue. The effectiveness of this new strategy was demonstrated by synthesizing six Aid-containing analogues of angiotensin-(1-7) on solid support. The Aid analogues of angiotensin-(1-7) exhibited increased peptidase stability against human ACE and DPP3 and improved anti-inflammation and antiproliferation activity.