Self-assembled molecular structures immobilized on solidsubstrates and composed of fluorophore-tagged oligonucleotide probes and an optical polymeric transducerwere investigated for the trace level detection of DNAtarget molecules. Rapid and efficient energy transferbetween the polymeric transducer and fluorophores withinthe molecular aggregates leads to a massive intrinsicamplification of the fluorescence signal and to the label-free detection of as little as 300 DNA molecules, with thespecificity required for the detection of single-nucleotidemismatches. This capacity for attomolar detection levelswhile the sensing structures are attached onto solidsupports could lead to the development of biochip platforms for fast and simple PCR-free multitarget DNAdetection.