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A <jats:italic>de novo<\/jats:italic> designed PEGylated heptapeptide\/aggregation\u2010induced emission (AIE) dye and MRI probe\u2010conjugated multimodal contrast agent, PEG\u2010AIE\u2010Pra\u2010Lys(DOTAGd<jats:sup>3+<\/jats:sup>)\u2010Lys(DOTAGd<jats:sup>3+<\/jats:sup>)\u2010Arg\u2010Gly\u2010Asp\u2010Ser, is synthesized employing the Fmoc\u2010solid phase peptide synthesis approach on Rink amide AM resin. In the heptapeptide sequence, two preorganized macrocyclic Lys(DOTAGd<jats:sup>3+<\/jats:sup>) chelates with a substantial magnetic moment (7.49 BM per Gd<jats:sup>3+<\/jats:sup>) are incorporated for MRI and integrated with an AIE probe for fluorescence imaging. PEGylation is achieved through PEG\u2010N<jats:sub>3<\/jats:sub> and the alkyne\u2010bearing N\u2010terminal amino acid L\u2010propargylglycine (Pra) via click chemistry, which enhances water solubility and circulation lifetime. The multifunctional PEGylated heptapeptide self\u2010assembles into magnetic nanovesicles in water, facilitating passive targeting of cancer cells. The C\u2010terminal RGDS residue enables active targeting of the cancer cell surface overexpressed receptor \u03b1<jats:sub>V<\/jats:sub>\u03b2<jats:sub>3<\/jats:sub> integrin, facilitating preferential delivery of both magnetic and AIE agents to the cancer site. This multifunctional contrast agent is used for live cancer cell\u2010targeted fluorescence confocal imaging in combination with MRI and exhibits a decent longitudinal relaxation rate (<jats:italic>r<\/jats:italic><jats:sub>1<\/jats:sub>) of 4.0305 mM<jats:sup>\u22121<\/jats:sup> s<jats:sup>\u22121<\/jats:sup>. Water\u2010soluble, biologically compatible, noncytotoxic, AIE\u2010tethered, macrocyclic Lys(DOTAGd<jats:sup>3+<\/jats:sup>) chelates comprising PEGylated paramagnetic nanovesicles of PEG\u2010AIE\u2010Pra\u2010Lys(DOTAGd<jats:sup>3+<\/jats:sup>)\u2010Lys(DOTAGd<jats:sup>3+<\/jats:sup>)\u2010Arg\u2010Gly\u2010Asp\u2010Ser serves as an effective multifunctional contrast agent for cancer\u2010targeted multimodal imaging applications.<\/jats:p>","DOI":"10.1002\/smll.202504502","type":"journal-article","created":{"date-parts":[[2025,7,9]],"date-time":"2025-07-09T15:44:17Z","timestamp":1752075857000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Design of Water\u2010Soluble PEGylated Heptapeptide\u2010Based Multifunctional Magnetic Nanovesicles for Cancer Targeted MRI Integrated With Fluorescence 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