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However, a quantitative framework linking molecular organization with nonlinear interfacial mechanics remains elusive. Here, we establish an analytical framework that captures the nonlinear elastic response of lipid\u2010membrane\u2010coated synthetic cells under micropipette aspiration. Incorporating both area stretching and curvature bending enables the model to quantitatively reproduce the complete pressure\u2010displacement response within the small\u2010deformation regime. This approach reduces interfacial mechanics to two parameters: the in\u2010plane area\u2010stretching modulus and an out\u2010of\u2010plane bending\u2010related term. Using this unified framework, we experimentally demonstrate that nonlinear interfacial mechanics can be programmed by altering the molecular geometry and effective dimensionality of adsorbed elements. The lipid molecular shape and curvature\u2010dependent packing regulate in\u2010plane stiffness, whereas DNA nanostructures, the other adsorbed element, introduce an orthogonal control axis via dimensionality: three\u2010dimensional network architectures markedly reinforce bending resistance. Together, these results establish a general molecular design principle for programming interfacial mechanics and provide a quantitative foundation for engineering mechanically tunable synthetic cells and soft interfaces.<\/jats:p>","DOI":"10.1002\/smsc.70321","type":"journal-article","created":{"date-parts":[[2026,6,16]],"date-time":"2026-06-16T13:20:09Z","timestamp":1781616009000},"source":"Crossref","is-referenced-by-count":1,"title":["Programming Nonlinear Interfacial Mechanics of Synthetic Cells: Lipid Geometry and DNA Nanostructures"],"prefix":"10.1002","volume":"6","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-9733-7894","authenticated-orcid":false,"given":"Kazutoshi","family":"Masuda","sequence":"first","affiliation":[{"name":"Komaba Institute for Science Graduate School of Arts and Sciences The University of Tokyo  Tokyo 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