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This review examines the structure\u2013activity relationships (SAR) of these peptides, focusing on how key structural features\u2014including disulfide connectivity, loop architecture, charge distribution, and backbone cyclization\u2014govern their biological activity, selectivity, and toxicity. Representative peptide families such as cyclotides, defensins, thionins, and snakins are discussed to highlight conserved structural motifs alongside variable regions that contribute to functional diversity. We further explore rational design and engineering strategies, including loop grafting, cyclization, charge modulation, and backbone stabilization, supported by selected case studies demonstrating improved pharmacological profiles, membrane interactions, and target specificity. Building on these insights, we propose a design\u2010oriented framework that integrates SAR\u2010guided peptide engineering with experimental toxicology and pharmacological evaluation to facilitate the development of plant\u2010derived peptides as therapeutic leads and molecular tools. This peptide\u2010centric perspective aims to complement existing studies on plant bioactive peptides and to advance the rational design of next\u2010generation peptide\u2010based therapeutics.<\/jats:p>","DOI":"10.1002\/psc.70132","type":"journal-article","created":{"date-parts":[[2026,9,26]],"date-time":"2026-09-26T06:51:25Z","timestamp":1790405485000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Structure\u2013Activity Relationships and Rational Engineering of Plant Defense and Toxic Peptides"],"prefix":"10.1002","volume":"32","author":[{"given":"Uyen N. 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