A novel adsorbent was fabricated by covalently anchoring N-(3-Nitro-benzylidene)-N'-trimethoxysilylpropylethane-1, 2-diamine onto multiwalled carbon nanotubes (NBATSPED-MWCNTs). This novel material was characterized by different techniques such as XRD, SEM, FT-IR and TGA-DTA. Subsequently, it was used for the ultrasound-assisted removal of aluminum (III) ions via its complexation with eriochrome cyanine R (ECR)indicator. The influences of variables such as initial ECR concentration (X 1 ), initial Al 3+ ions concentration (X 1 ), adsorbent dosage (X 3 ) and contact time (X 4 ) on the efficiency of removal process were investigated by small central composite design (CCD) under response surface methodology and genetic algorithm (GA). The process was empirically modeled to reveal the significant variables and their possible interactions. The optimization conditions were set as: 3 min, 20.238 mg, 20 mg L -1 and 15 mg L -1 for sonication time, adsorbent mass, initial Al 3+ ions concentration and initial ECR concentration, respectively. Finally, it was found that the equilibrium and kinetic of adsorption process follow the Langmuir isotherm and pseudo-second-order kinetic model, respectively. From the Langmuir isotherm, maximum monolayer capacity (q max ) was obtained to be 46.74 mg g −1 at optimum conditions.