A novel development on halloysite-polyvinyl alcohol (HNTs-PVA) nanocomposites has been conducted using malonic acid (MA) by crosslinking PVA and HNTs. PVA-MA crosslinking produces smooth surfaces, which play an important role in enhancing the properties of HNTs-PVA nanocomposite. The crystallographic structures of crosslinked HNTs-PVA show almost no change as depicted by the X-ray diffraction (XRD)-2θ-peak, suggesting that MA has no or little influence on the crystallographic structure of the HNTs-PVA. Images taken by field emission scanning electron microscope (FESEM) suggest possible effects of MA on the morphology and internal features of HNTs-PVA by reducing the agglomeration of HNTs, which is considered a decisive step in improving the surface qualities of HNTs. Investigating the samples using the Brunauer-Emmelt-Teller (BET) technique showed that the surface area was increased by about 10 times, reaching the second highest recorded results compared to the HNTs, which could be considered a breakthrough step in enhancing the properties of HNTs-PVA due to MA crosslinking.