Currently, adsorbents with high adsorption performance for eliminating pollutants from discharged wastewater have received many researchers’ attention. To this aim, a novel AMXGO absorbent was fabricated by intercalating graphene oxide (GO) into alkalized MXene (Alk-MXene) layer which exhibited high efficacy for the removal of cationic Malachite Green (MG) and anionic Congo Red (CR). Analysis of FTIR, XRD, SEM and TG presented that AMXGO absorbent have a typical three-dimensional layer by layer structure and abundant oxygen-containing groups and its thermal stability was remarkably improved. BET results elucidated that AMXGO1 adsorbent has larger specific surface area and pore volume (16.686 m2 g−1, 0.04733 cm3 g−1) as compared to Alk-MXene (4.729 m2 g−1, 0.02522 cm3 g−1). A dependence of adsorption performance on mass ratio between Alk-MXene and GO, initial dye concentration, contact time, temperature and pH was revealed. Maximum adsorption capacity of MG (1111.6 mg/g) and CR (1133.7 mg/g) were particularly found for AMXGO1 absorbent with a mass ratio of 3:1 and its removal for both dyes were higher than 92%. The adsorption process of AMXGO1 adsorbent for both MG and CR complies with pseudo-second-order kinetic model and Freundlich isotherm model. In addition, adsorption mechanism was explored that synergism effects as electrostatic attraction, π-π conjugates, intercalation adsorption and pore filling were the main driving force for the high adsorption performance of dye. Therefore, AMXGO adsorbent has a potential application prospect in the purification of dye wastewater.