Four new organically templated molybdenum compounds, (C4H12N2)[MoO2(H2AsO4) (AsO4)] (1), (C4H12N2)[MoO2(H2PO4)(PO4)]·H2O (2), (C4H12N2)[MoO2(C2O4)(HAsO4)] (3), and (C6H14N2)3[(MoO2)4(C2O4)4(H2PO4)2]·8.5H2O (4), have been prepared under mild hydrothermal conditions and characterized by single-crystal X-ray diffraction and thermogravimetric (TG) analysis. All four structures are one-dimensional and contain diprotonated amine cations. The first three compounds are the first organically templated chain structures in the MoVI/X/O (X = As, P) lattices; 3 and 4 are the first inorganic−organic mixed anion materials in the molybdenum arsenate and phosphate systems, respectively. Crystal data: 1, monoclinic, P21/n, a =13.4544(8) Å, b = 6.5648(4) Å, c = 14.6312(8) Å, β = 107.522(1)°, Z = 4; 2, triclinic, P-1, a = 6.4249(3) Å, b = 8.6860(4) Å, c = 12.4506(6) Å, α = 80.539(1)°, β = 75.140(1)°, γ = 70.161(1)°, Z = 2; 3, monoclinic, P21/n, a = 6.4577(2) Å, b = 13.0135(3) Å, c = 15.3606(2) Å, β = 93.199(1)°, Z = 4; 4, triclinic, P-1, a = 8.6384(1) Å, b = 17.7583(3) Å, c = 18.1172(3) Å, α = 97.979(1)°, β = 102.441(1)°, γ = 98.830(1)°, Z = 2. Both crystals of 1 and 2 contain the double [Mo2X2O12(H2XO4)]∞ ribbon, which can be derived from that of VO(HPO4)·4H2O. Introduction of oxalate anions into the reaction results in 3 and 4, which contain unusual [MoAsO6(C2O4)]∞ and [Mo2PO8(C2O4)2]∞ chains, respectively. According to the results of TG and DT analyses, the structural motifs of 1, 3, and 4 are thermally stable up to ∼250 °C.