In this study, two types of carbon nanotube (CNT) modified surfaces for the attachment of Bacillus anthracis spores were examined. Multi-walled carbon nanotube (MWCNT) forest on silicon wafer and MWCNT sheet on poly(methyl methacrylate) (PMMA) film were used. Both types of MWCNT surfaces significantly increased surface hydrophobicity (P < 0.05) and increased the attachment of spores on their surfaces compared to the uncoated substrates, respectively. However, no inhibitory effect was observed on the germination of attached spores on both types of MWCNT surfaces. MWCNT-coated surfaces showed the potential as adsorbents for removal of Bacillus spores from fluids.