The surface plasmon modes of metal nanoparticles provide a way to efficiently enhance the excitation and emission from a fluorescent dye. We have employed DNA-directed assembly to prepare dimers of gold nanoparticles and used their longitudinally coupled plasmon mode to enhance the fluorescence emission of an organic red-emitting dye, Atto-655. The plasmon-enhanced fluorescence of this dye using dimers of 80 nm particles was measured at the single-molecule detection level. The top enhancement factors were above 1000-fold in 71% of the dimers within a total of 32 dimers measured, and in some cases, they reached almost 4000-fold, in good agreement with model simulations. Additionally, fluorescence lifetime correlation analysis enabled the separation of enhanced from nonenhanced emission simultaneously collected in our confocal detection volume. This approach allowed us to recover a short relaxation component exclusive to enhanced emission that is attributed to the interaction of the dye with DNA in the interparticle gaps. Indeed, the frequency of enhancement events is larger than that expected from the volume occupancy of the gap region, thus suggesting that the interaction of the dye with DNA linkers favors the observation of emission enhancement in our dimer particles.