Raman spectra of aqueous solutions containing up to 40 mol% of formaldehyde were recorded in the 120-4000 cm-1 spectral range. The water vibrational modes are not too heavily modified by the presence of the polymerized species in the aqueous solutions. The intensity of the bands corresponding to the C-O and C-H vibrational modes depends on the water content. Two bands are found for the C-O symmetric and antisymmetric stretching modes. The first is related to the C-O-C groups formed within the oligomer chains as the condensation increases and the second to the C-OH groups located at the end of the oligomer chains. A change in the intensity evolution of the bands corresponding to the stretching modes of the C-O-C groups occurs above 15 mol% formaldehyde concentration, corresponding to the formation of the HO(CH2O)nH oligomers with n3. The intensity of the stretching modes due to the C-OH groups varies linearly with concentration. A linear variation of the band intensity of the CH modes as a function of formaldehyde content is also observed. Copyright © 2003 John Wiley & Sons, Ltd