Three lipid-oligonucleotides (ODN) carrying TEMPO were prepared and formed a micelle with a diameter of ca. 10 nm. The double strand ODN, lipid-polyTinDS, incorporating TEMPO near the core of the micelle showed the largest water-proton relaxivity, r1, value of 2.4 (25 MHz, 0.59 T) and 6.8 mM−1 s−1 (42 MHz, 1.0 T) per TEMPO.