Hybrid carbon nanotubes (CNTs) are grown on biomass powder-activated carbon (bio-PAC) by loading iron nanoparticles (Fe) as catalyst templates using chemical vapor deposition (CVD) and using acetylene as carbon source, under specific conditions as reaction temperature, time, and gas ratio that are 550 °C, 47 min, and 1, respectively. Specifications of hybrid CNTs were analyzed and characterized using field emission scanning electron microscope (FESEM) with energy-dispersive X-ray spectroscopy (EDX), transmission electron microscopic (TEM), Fourier-transform infrared (FTIR), X-ray diffraction (XRD), thermogravimetric analysis (TGA), surface area Brunauer–Emmett–Teller (BET), and zeta potential. The results revealed the high quality and unique morphologies of hybrid CNTs. Furthermore, removal and capacity of Al3+ were optimized by response surface methodology (RSM). However, the results revealed that the pseudo-second-order model well represented adsorption kinetic data, while the isotherm data were effectively fitted using a Freundlich model. The maximum adsorption capacity was 347.88 mg/g. It could be concluded that synthesized hybrid CNTs are a new cost-effective and promising adsorbent for removing Al3+ ion from wastewater.