Orange-red transparent single crystals of LiEu2(NCN)l(3) and LiEU4(NCN)(3)l(3) were synthesized from fluxes of europium iodide, sodium cyanide, sodium azide, and lithium iodide at elevated temperatures and structurally characterized by X-ray diffraction. While LiEu2(NCN)l(3) crystallizes in the cubic system (Fd (3) over barm, a = 15,1427(17) Angstrom, V = 3472.2(7) Angstrom(3), Z = 16, R1 = 0.0322), LiEu4(NCN)(3)l(3) adopts the hexagonal system (P6(3)/mmc, a = 10.6575(11) Angstrom, c = 6.8232(10) Angstrom, V = 671.16(14) Angstrom(3), Z = 2, R1 = 0.0246). Both extended structures are composed of complex frameworks built from europium tetrahedra coordinated by carbodiimide (symmetrical NCN2-) units on the one side and condensed iodine octahedra around lithium cations on the other. Within LiEu2(NCN)l(3), vertex-sharing of the Lil(6) subunits together with isolated europium tetrahedra results in two three-dimensional networks interpenetrating each other. Within LiEu4(NCN)(3)l(3), face-sharing of the europium tetrahedra results in bitetrahedral units which further connect via two opposing vertexes into one-dimensional linkages. Likewise, the Lil(6) octahedra share common faces to also yield one-dimensional linkages that fill the channels between the europium/carbodiimide substructure. The magnetic behavior of both compounds has been determined; the two phases follow Curie-Weiss laws with weak predominantly ferromagnetic exchange between the europium ions and atomic moments characterizing them as essentially divalent.