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The development of artificial vesicles into responsive architectures capable of sensing the biological environment and simultaneously signaling the presence of a specific target molecule is a key challenge in a range of biomedical applications from drug delivery to diagnostic tools. Herein, the rational design of biomimetic DNA-grafted quatsome (QS) nanovesicles capable of translating the binding of a target molecule to amphiphilic DNA probes into an optical output is presented. QSs are synthetic lipid-based nanovesicles able to confine multiple organic dyes at the nanoscale, resulting in ultra-bright soft materials with attractiveness for sensing applications. Dye-loaded QS nanovesicles of different composition and surface charge are grafted with fluorescent amphiphilic nucleic acid-based probes to produce programmable FRET-active nanovesicles that operate as highly sensitive signal transducers. The photophysical properties of the DNA-grafted nanovesicles are characterized and the highly selective, ratiometric detection of clinically relevant microRNAs with sensitivity in the low nanomolar range are demonstrated. The potential applications of responsive QS nanovesicles for biosensing applications but also as functional nanodevices for targeted biomedical applications is envisaged., This work was financially supported by the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska- Curie grant agreement “Nano-Oligo Med” (No 778133), Ministry of Science and Innovation (MINECO), Spain, through the “MOL4BIO” project (PID2019-105622RB-I00) and by Instituto de Salud Carlos III (DTS20/00018), Italian Ministry of University and Research (Project of National Interest, PRIN, 2017Y2PAB8_004 through the project “Cutting Edge Analytical Chemistry Methodologies and Bio-Tools to Boost Precision Medicine in Hormone-Related Diseases”. M.R. was supported from a Fondazione Umberto Veronesi postdoctoral fellowship. Furthermore, ICMAB-CSIC acknowledges support from the MINECO through the Severo Ochoa Programme for Centers of Excellence in R&D (SEV-2015-0496 and CEX2019-000917-S). Quatsome production and their physicochemical characterization has been performed by the Biomaterial Processing and Nanostructuring Unit (U6) of the ICTS “NANBIOSIS”, a unit of the CIBER network in Bioengineering, Biomaterials & Nanomedicine (CIBER-BBN) located at the Institute of Materials Science of Barcelona (ICMAB-CSIC).