A new type of DTPA-bis-amides (L1-L4) and their Gd(III)-complexes of the type $[Gd(L)(H_2O)]{cdot}nH_2O$ (5: L1; 6: L2; 7: L3; 8: L4) have been prepared and characterized by analytical and spectroscopic techniques. The X-ray crystal structure of 8 has been determined for structural confirmation. The coordination geometry adopts a tricapped trigonal prism geometry with L4 acting as a chelate octadentate and a water molecule in the coordination sphere. Crystals are monoclinic, $P2_1$, a = 14.468(3), b = 19.235(4), c = 13.527(2) $AA$ $eta$ = $107.245(3)^{circ}$, V = 3595.2(11) $AA^3$, Z = 4, $D_{calc}$ = 1.570. Significant increases in relaxivities are observed with 6 and 7 as compared with that of $Omniscan^{(R)}$, a commercial MR agent: R1 = 12.46 $mM^{-1};s^{-1}$, R2 = 8.76 $mM^{-1};s^{-1}$ for 6; R1 = 12.77 nm-1 s-1, R2 = 7.60 mM-1 s-1 for 7; R1 = 4.9 $mM^{-1};s^{-1}$, R2 = 4.8 $mm^{-1};s^{-1}$ for $Omniscan^{(R)}$. In the case of 5, however, both R1 and R2 are found to be lower to show 2.09 $mM^{-1};s^{-1}$, and 1.82 $mM^{-1};s^{-1}$, respectively.