In this study, the effects of a coupling agent and additive on the physicomechanical (morphological, mechanical, thermal, and swelling) properties of tea dust (TD)–polypropylene (PP) composites were studied. TD–PP composites were prepared with untreated tea dust (UTD) and tetraethylsilane (TES)‐treated TD or silanated tea dust (STD) particles at ratios of 0:100, 10:90, 20:80, 30:70, and 40:60 w/w. Initially, TD particles were grafted by TES as a coupling agent, and these STD particles were then modified with graphene oxide (GO) as an additive to study their effects on the STD–PP composites; these were compared to the STD–PP and UTD–PP composites in accordance with a study of improvements in the mechanical properties. All of the TD–PP composites were analyzed with Fourier transform infrared spectroscopy, scanning electron microscopy, and mechanical, thermal, and physical tests. The thermal and mechanical properties of both the STD–PP and GO‐modified STD–PP composites were found to be improved as compared to those of the UTD–PP composites. So, the recycling of a large amount of TD as a waste material could be useful in the preparation of TD–PP composites. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016, 133, 42927.