CdTe nanocrystals have been synthesized in aqueous solution at 92oC under open-air conditions. During the reaction, aliquots of the samples were taken at different growth times and used to obtain their UV-Vis absorbance and photoluminescence spectra in order to estimate the nanocrystal size. The absorption peaks are located around 459 nm for 1 h, 478 nm for 2 h, 491 nm for 4 h, 532 nm for 7 h and 610 nm for 94 h of growth time. The mean nanocrystal size for these samples is 2 nm, 2.2 nm, 2.3 nm, 2.6 nm and 3.4 nm, respectively, according to the theoretical calculations of 1s1/2 – 1s3/2 excitonic transition. Finally, CdTe nanocrystals were assembled using layer-by-layer technique on glass substrates, using PDDA as cationic polyelectrolyte and negatively charged CdTe nanocrystals. The Raman spectroscopy shows that CdTe nanocrystals preserve the nanoparticle properties after being assembled.