This study demonstrates the feasibility of applying free-breathing, cardiac-gated, susceptibility-weighted fast spin-echo imaging together with black blood preparation and navigator-gated respiratory motion compensation for anatomically accurate T2* mapping of the heart. First, T2* maps are presented for oil phantoms without and with respiratory motion emulation T2* = (22.1 +/- 1.7) ms at 1.5 T and T2* = (22.65 +/- 0.89) ms at 3.0 T). T2* relaxometry of a ferrofluid revealed relaxivities of R2* = (477.9 +/- 17) mM(-1)s(-1) and R2* = (449.6 +/- 13) mM(-1)s(-1) for UFLARE and multiecho gradient-echo imaging at 1.5 T. For inferoseptal myocardial regions mean T2* values of 29.9 +/- 6.6 ms (1.5 T) and 22.3 +/- 4.8 ms (3.0 T) were estimated. For posterior myocardial areas close to the vena cava T2*-values of 24.0 +/- 6.4 ms (1.5 T) and 15.4 +/- 1.8 ms (3.0 T) were observed. The merits and limitations of the proposed approach are discussed and its implications for cardiac and vascular T2*-mapping are considered.