The poly(ethylene terephthalate) waste was depolymerized using 1,4-butanediol, and diethylene glycol and the glycolyzed products were used in the preparation of the unsaturated polyester. The composition of the glycolyzed products and the prepared polyester (unsaturated polyester) were investigated in view of their infrared and 1 H NMR spectra. Different samples of unsaturated polyester/nanocomposites containing various amounts (1, 3, and 5 wt%) of different nanofillers, namely Nanofil 116, Cloisite 30B, and Laponite RD, were also prepared. The effect of the nanofiller type and content on the morphological structure of the fractured surfaces, thermal, mechanical, and electrical properties was investigated.