Abstract: | The pH‐dependent self‐assembling of gold nanoparticles is described. Oligonucleotides containing four or six consecutive dC residues are immobilized on 15‐nm gold nanoparticles. Their assembly is based on the formation of a DNA i‐motif as determined by the color change from red to blue between pH 5.5 and 6.5. The process occurs within a narrow pH range and is reversible. The i‐motif is formed by the antiparallel intercalation of two parallel duplexes provided by two different gold nanoparticles. This assembly process can be utilized to generate novel systems for colorimetric sensing, applications in medical imaging and therapy, and for the construction of a proton‐driven nanomachine. |