Carbon Nanotubes (CNTs) are known for effective adhesion, growth, and differentiation of bone, muscle, and cardiac cells. CNTs can provide excellent mechanical and electrical properties for cell scaffolding; however, loose CNTs can cause in-vivo toxicity. To suppress this risk, our team has developed biomimetic scaffolds with multiscale hierarchy where carpet-like CNT arrays are covalently bonded to larger biocompatible substrates. In this study, we investigated the interaction between glioblastoma multiforme (GBM) cells (U87MG) and our unique hierarchical CNT-coated scaffolds upon brain tumor cell proliferation. U87MG cells grown on un-modified carbon scaffolds grew in a bi-phasic fashion. Initially, the scaffolds prevented GBM cell growth; however, prolonged growth on such scaffolds significantly increased GBM cell proliferation. We further defined the importance of the hydrophobicity/hydrophilicity of the CNT-coated scaffolds in this cellular response by utilizing sodium-hypochlorite based bleach treatment prior to cellular exposure. This surface modification increased the hydrophilicity of the CNT-coated scaffolds and ameliorated the biphasic response of U87MG cells allowing for a normal growth curve. Findings highlight the importance of surface modification and wettability of the CNT-coated scaffolds for cell growth applications. The focus for this study was to determine whether scaffold surface features could modulate tumor-scaffold interactions, and thus to improve our understanding of and optimize successful development of future scaffold-based chemotherapy applications. Overall, it appears that the wettability of carbon scaffolds coated with CNTs is an important regulator of U87MG cellular growth. These findings will be important to consider when developing a potential chemotherapy-attached implant to be used post-surgical resection for GBM patient treatment.