In this paper, the effect of pH and temperature on the structure of urea-formaldehyde resins was studied. GPC, NMR and Raman measurements were performed to elucidate the structural characteristics of the resin systems. Fourier Transform Near Infrared (FT-NIR) spectroscopy via optical fibers was used to monitor the reaction progress in situ. It was found that the reactions of urea and formaldehyde at different temperatures and pH values result in resins with different structures and properties: Resins produced at high temperatures and acidic pH values exhibit higher degrees of condensation, presumably because of the development of more cross-linked structures.