This study provides a detailed investigation into the chemical grafting of multiwalled carbon nanotubes (MWNTs) with starch at various concentrations and reaction temperatures. Utilizing Raman spectroscopy and Fourier-transform infrared spectroscopy (FTIR), we identified structural defects in the MWNTs and characterized the functional groups introduced by the grafting process. Differential scanning calorimetry (DSC) and thermogravimetric analysis (TGA) deepened our understanding of the interactions between starch and MWNTs, and quantified the polysaccharide content. Transmission electron microscopy (TEM) unveiled nanostructures arising from the interplay between MWNTs and starch molecules. Our findings highlight the potential of starch-grafted MWNTs for applications in nanotechnology and nanomedicine, positioning them as a promising material for targeted drug delivery and tissue engineering, aligning with Nano LIFE’s multidisciplinary goals in life sciences, nanosciences and nanomedicine.