The redox reactions of various lanthanide metals with 3-(4-pyridyl)pyrazole (4-PyPzH) or 3-(3-pyridyl)pyrazole (3-PyPzH) ligands yield the 2D network 2∞[Eu(4-PyPz)2(Py)2] containing divalent europium, the 3D frameworks 3∞[Ln(4-PyPz)3] and 3∞[Ln(3-PyPz)3] for trivalent cerium, praseodymium, neodymium, holmium, erbium, and thulium as well as 3∞[La(4-PyPz)3], and the 2D networks 2∞[Ln(4-PyPz)3(Py)] for trivalent cerium and thulium and 2∞[Ln2(4-PyPz)6]·Py for trivalent ytterbium and lutetium. The 18 lanthanide coordination polymers were synthesized under solvothermal conditions in pyridine (Py), partly acting as a co-ligand for some networks. The compounds exhibit a variety of luminescence properties, including metal-centered 4f–4f/5d–4f emission in the visible and near-infrared spectral range, metal-to-ligand energy transfer, and ligand-centered fluorescence and phosphorescence. The anionic ligands 3-PyPz− and 4-PyPz− serve as suitable antennas for lanthanide-based luminescence in the visible and near-infrared range through effective sensitization followed by emission through intra–4f transitions of the trivalent thulium, holmium, praseodymium, erbium, and neodymium. 2∞[Ce(4-PyPz)3(Py)], 3∞[Ce(4-PyPz)3], and 3∞[Ce(3-PyPz)3] exhibit strong degrees of reduction in the 5d excited states that differ in intensity compared to the ligand-based emission, resulting in a distinct emission ranging from pink to orange. The direct current magnetic studies show magnetic isolation of the lanthanide centers in the crystal lattice of 3∞[Ln(3-PyPz)3], Ln = Dy, Ho, and Er.