Nanobiomaterials based on superhydrophilic vertically-aligned multi-walled carbon nanotubes (VAMWCNT-O2) are promising for their properties and bone tissue biocompatibility. VAMWCNT-O2 films with nanohydroxyapatite (nHAp) aim to improve mechanical properties and biocompatibility of this new nanocomposite due to its resemblance to bone matrix structure. This study aimed to produce in vitro biomineralized nHAp/VAMWCNT-O2 nanocomposites using simulated body fluid (SBF) with two different pHs (6.10 and 7.40) during 7 days to obtain a new surface design with higher crystalinity and better morphology of nHAp/VAMWCANT-O2 nanocomposites. The objective is to obtain biomineralized nanobiomaterials to enable its applicability as "scaffold" to cellular support and consequent bone tissue formation, accelerating the osseointegration. Layer densification has been achieved due to polycrystalline nanoapatites deposition on surface and between the biomineralized nHAp/VAMWCNT-O2 nanocomposites, without any heat treatment. Therefore, through its characteristics and properties these nanocomposite applications can be considered extremely viable for acceleration of in vivo regenerative processes.