In an effort towards the visualization of b-amyloid (Ab) plaques by T1-weighted magnetic resonance imaging for detection of Alzheimer’s disease, we report the synthesis and characterization of stable, noncharged Gd3? complexes of three different 1,4,7,10- tetraazacyclododecane-1,4,7-triacetic acid monoamide derivatives conjugated to Pittsburgh compound B, a wellestablished marker of Ab plaques. The ligands L1, L2, and L3 differ in the nature and size of the spacer linking the macrocyclic chelator and the Pittsburgh compound B targeting moiety, which affects their lipophilicity, the octanol– water partition coefficients of the complexes ranging from -0.15 to 0.32. Given their amphiphilic behavior, the complexes form micelles in aqueous solution (critical micellar concentration 1.00–1.49 mM). The parameters determining the relaxivity, including the water exchange rate and the rotational correlation times, were assessed for the monomeric and the micellar form by a combined 17O NMR and 1H nuclear magnetic relaxation dispersion (NMRD) study. They are largely influenced by the aggregation state and the hydrophobic character of the linkers. The analysis of the rotational dynamics for the aggregated state in terms of local and global motions using the Lipari– Szabo approach indicates highly flexible, large aggregates. On binding of the complexes to human serum albumin or to the amyloid peptide Ab1–40 in solution, they undergo a fourfold and a twofold relaxivity increase, respectively (40 MHz). Proton relaxation enhancement studies confirmed moderate interaction of Gd(L1) and Gd(L3) with human serum albumin, with KA values ranging between 250 and 910 M-1. ; This work was financially supported by Fundação para a Ciência e a Tecnologia, Portugal (PhD grant SFRH/BD/ 46370/2008 to AFM) and Rede Nacional de RMN (project REDE/ 1517/RMN/2005) for the acquisition of the Varian VNMRS 600 NMR spectrometer in Coimbra and the French-Portuguese PESSOA project. This work was carried out in the frame of the European Actions TD1004 ‘‘Theragnostics Imaging and Therapy’’ and TD1007 ‘‘PET-MRI’’.