Hyphenation of thermogravimetric analyzer (TGA) and thermo-Raman spectrometer for in situ investigation of thermal decomposition of Zn(CH3COO)(2)(.)2H(2)O forming ZnO nanoparticles (diameter similar to50 nm), using oxygen as carrier gas is executed simultaneously. Influence of carrier gas flow rate forming thin films is also investigated. The thermo-Raman spectra recorded at every degree interval could follow the intermediates formed. The thermo-Raman intensity thermograms of the characteristic bands provided information of the decomposition pathway and mechanism, and are supported by complementary characterizations using SEM, TEM, EDS, FT-IR, and XRD. (C) 2003 Elsevier B.V. All rights reserved.