Three lipid-oligonucleotides (ODN) carrying TEMPO were prepared and formed a micelle with a diameter of ca. 10 nm. The double strand ODN, lipid-polyT in DS, incorporating TEMPO near the core of the micelle showed the largest water-proton relaxivity, r 1 , value of 2.4 (25 MHz, 0.59 T) and 6.8 mM 21 s 21 (42 MHz, 1.0 T) per TEMPO.DNA derivatives carrying stable aminoxyls through various types of linkers have previously been prepared, revealing not only the conformation of various DNA strands but also their dynamics. 1 Such DNA double strands carrying organic spins could be expected to function as metal-free and large-size MRI agents, 2 taking advantage of the unique properties of the DNA strand, which binds to many water molecules in major and minor grooves for structural stabilization. 3 Recently, we reported that the double strand incorporating 5-uridine-TEMPO, UST, had relatively large water-proton relaxivity, r 1 , which is an indicative value for the contrast. 4 To increase the molecular size and further improve of the r 1 value, in this study DNA-micelles 5 carrying TEMPO, 2,2,6,6tetramethylpiperidine-N-oxyl, were prepared. The 15-mer of thymidine (polyT) and TEMPO-uridine (TDU) directly attached to the TEMPO radical without a linker, were selected as the base sequence and a spin source, respectively. We report the rotational correlation time, t R , and the relaxivities, r 1 , for their single-strand and double-strand micelles with complimentary strand (polyA), in addition to T 1 -weighted images in vitro (Fig. 1).The TDU monomer, was prepared by Suzuki coupling reaction; 5-iodo-29-deoxyuridine reacted with 4-borate TEMPO in the presence of tetrakis(triphenylphosphine)palladium(0). After pro-