P-nitroaniline (PNA) is an aniline compound with high toxicity and can cause serious harm to aquatic animals and plants. Multiwalled carbon nanotubes (MWCNTs) are a multifunctional carbon-based material that can be applied in energy storage and biochemistry applications and semiconductors as well as for various environmental purposes. In the present study, MWCNTs (CO2–MWCNTs and KOH–MWCNTs) were obtained through CO2 and KOH activation. ACID–MWCNTs were obtained through surface treatment with an H2SO4–HNO3 mixture. Herein, we report, for the first time, the various MWCNTs that were employed as nanoadsorbents to remove PNA from aqueous solution. The MWCNTs had nanowire-like features and different tube lengths. The nanotubular structures were not destroyed after being activated. The KOH–MWCNTs, CO2–MWCNTs, and ACID–MWCNTs had surface areas of 487, 484, and 80 m2/g, respectively, and pore volumes of 1.432, 1.321, and 0.871 cm3/g, respectively. The activated MWCNTs contained C–O functional groups, which facilitate PNA adsorption. To determine the maximum adsorption capacity of the MWCNTs, the influences of several adsorption factors—contact time, solution pH, stirring speed, and amount of adsorbent—on PNA adsorption were investigated. The KOH–MWCNTs had the highest adsorption capacity, followed by the CO2–MWCNTs, pristine MWCNTs, and ACID–MWCNTs. The KOH–MWCNTs exhibited rapid PNA adsorption (>85% within the first 5 min) and high adsorption capacity (171.3 mg/g). Adsorption isotherms and kinetics models were employed to investigate the adsorption mechanism. The results of reutilization experiments revealed that the MWCNTs retained high adsorption capacity after five cycles. The surface-activated and modified MWCNTs synthesized in this study can effectively remove hazardous pollutants from wastewater and may have additional uses.