The new chalcogenides CsCuNd2Se4 and CsCuGd2Te4 with analogous formulae were prepared from the elements by a flux method with CsCl as fluxing agent and cesium source. CsCuNd2Se4 crystallizes in the orthorhombic space group Cmcm (no. 63) with four formula units per unit cell (a = 424.69(3), b = 1475.81(8), c = 1465.42(8) pm), whereas CsCuGd2Te4 is monoclinic with the space group C2/m (no. 12) and twelve formula units per unit cell (a = 3764.75(19), b = 436.70(2), c = 2105.37(11) pm, β = 107.423(4)°). Both crystal structures feature three‐dimensional arrangements of the lanthanide and coinage metal cations along with the chalcogenide anions according to {}^3_\infty{[CuLn2Ch4]–} (Ln = Nd or Gd, Ch = Se or Te), leaving channels behind, in which the Cs+ cations are incorporated. Hereby, vertex‐linked [CuCh4]7– tetrahedra join to form {}^1_\infty{[CuCh3]5–} chains in both cases. Whereas for the CsCuNd2Se4 structure, these chains ({}^1_\infty{[CuSe3]5–}) are embedded into a three‐dimensional network, erected by edge‐ and vertex‐linked [NdSe6]9– octahedra, which form corrugated layers further connected by common edges, in CsCuGd2Te4 a different three‐dimensional {}^3_\infty{[Gd2Te4]2–} framework arises, comprising {}^1_\infty{[CuTe3]5–} chains, as well as vertex‐ and edge‐linked [GdTe6]9– octahedra. The major difference of the structures originates from the channels, in which the Cs+ cations are located. In the tunnels of CsCuNd2Se4, the Cs+ cations exhibit a bicapped trigonal prismatic selenide coordination, whereas in CsCuGd2Te4 with two Cs+ cations in one channel, they show bicapped trigonal prisms, as well as monocapped cubes of telluride anions as coordination spheres.