A series of new near-infrared (NIR) luminescent lanthanide-quinolinate derivatives [Ln(Q-Si)(3)] and xerogels (named as LnQSi-Gel, Ln = Er, Nd, Yb) covalently linked with the Ln(Q-Si)(3) by using the 8-hydroxyquinoline-functionalized alkoxysilane (Q-Si) have been synthesized. The obtained xerogel materials LnQSi-Gel are rigid and show homogeneous by field-emission scanning electron microscopy (FE-SEM) images. The Fourier-transform infrared (FT-IR), fluorescence spectra of Ln(Q-Si)(3), and LnQSi-Gel were measured, and the corresponding luminescence decay analyses were recorded. Of importance here is that the excitation spectra of the Ln(Q-Si)(3) and LnQSi-Gel extend to the region of visible light (more than 500 nm). Upon ligand-mediated excitation with the visible light, the Ln(Q-Si)(3) and LnQSi-Gel show the characteristic NIR-luminescence of the corresponding lanthanide ions through the intramolecular energy transfer from the ligands to the lanthanide ions. The good luminescent performances enable these NIR-luminescent xerogel materials to have possible applications in medical diagnostics, laser systems, and optics, etc.