The utilization of carbon nano-based materials in different applications acquired great attention in the last two decades, especially those related to environmental protection [
1‐
4]. The water contaminated with oil not only affects all life being organisms, but also decelerates the industrial revolutions. The discharged water coming out from different factories contains multiple contaminants like dyes and oil [
5]. The great challenges are not only separating oil from water but also removing other contaminants. The multi-function materials capable of performing multi-tasks are favored. The scientific society proposed different advanced techniques to clean up oil spills from water, such as coagulation and fluctuation, chemical oxidation, adsorption, biological treatment, photocatalytic treatment, and membrane technology [
6‐
8]. Among all of the separation techniques, membrane technology is favored. The membranes are durable and cost-effective, consume less energy, are single-stage, have corrosive resistance, and are non-toxic, environmentally friendly, and efficient [
9].
Due to their outstanding properties, sodium titanate nanotubes (TNTs) were subjected to massive research in past decades [
10]. The application areas of TNT comprise energy storage [
11‐
13], photocatalysis [
14], sensors [
14], dye removal [
15‐
17], and fire protection [
18]. Sodium titanate has a general Na
2Ti
nO
2n+1 (
n = 3–8) formula, with numerous crystalline phases with different physicochemical properties. Specifically, Na
2Ti
3O
7 and Na
2Ti
6O
13 have been comprehensively studied because of their exceptional stability and outstanding ionic conductivity [
10]. Several approaches like sol–gel, solid-state, and hydrothermal have been reported for TNT preparation [
19]. The hydrothermal method is a single-step process that produces many TNTs with different morphologies [
20]. Carbon nanotubes (CNTs) are promising 1D materials with splendid functionalities used in different fields [
21‐
23]. It was applied as a sensitive material to various physical, chemical, and biological stimuli; however, some limitations related to its intrinsic characteristics hinder its practical applications [
24‐
29]. It was reported that the incorporation of CNTs with some functional materials (e.g., metal oxides) resulted in enhancing the functionality of the resultant composite [
30,
31]. The incorporation of sodium titanate and CNTs was reported to have untraditional merits compared to their separate components. Payan et al., successfully synthesized TNT/SWCNT via a two-step hydrothermal route. The proposed composite was tested against 4-CP degradation under UV and solar irradiation [
32]. Santos et al., have prepared TNT/MWCNTs through the hydrothermal method. They concluded that the modification of TNT with MWCNTs led to a remarkable enhancement in the oxidization of methyl yellow (MY) [
33]. Mohamed et al., prepared MWCNTs/TNT nanocomposites loaded with platinum nanoparticles as methylene blue (MB) dye removal. Their research work demonstrated that the combination between TNT and MWCNT resulted in a superior photocatalytic activity in the degradation of MB [
34]. Jiang et al., synthesized CNT/TNT composite to be applied as photocatalyst material for methyl orange (MO) dye. According to their results, the degradation rate reached 94% after irradiation for 40 min. Hongchao Li et al., successfully prepared carbon membranes by the mixing polyacrylonitrile and phenolic resin via the pyrolysis process. They approached an optimal rejection for oil with 94.2% [
35]. Carbon membrane coated with polyethylene glutaraldehyde was prepared. The impacts of coating sorts and solutions used as well as the concentration for the structure and the separation efficiency for oily wastewater were explored while ~ 94% separation was affirmed in another report [
36]. Herein, through this work, titanium dioxide nanoparticles (TiO
2) were grown on the external surface of CNTs, and then transformed into TNT via a hydrothermal route. The earlier obtained composite was doped with nitrogen using a solid-state reaction followed by calcination. The main target of this study is to acquire a smart material having oil/water separation properties. The prepared composites were studied using different techniques including XRD, FTIR, UV–Vis, SEM, and HR-TEM, to assess their properties, and then tested for the application mentioned earlier. The microstructural-related parameters such as microstrain, dislocation density, and crystallinity degree were calculated from the XRD diffractograms. The conducted optical study reveals an interaction between the doped TNT and CNT. This interaction alters the energy level of the conduction band. The studied membrane was prepared using a simple vacuum filtration method. The efficiency of the synthesized membranes was investigated initially against n-hexane. The obtained results confirmed the sample CNTs-TNT1.0 has the highest separation efficiency. The latter was tested versus different oils.