Efficient removal of broad-spectrum organic pollutants is crucial in wastewater treatment. This research focuses on the synthesis of three-dimensional TiVCT X MXene/graphene nanosheet-based aerogels, known as TiVCT X /GAs, using a straightforward hydrothermal self-assembly method, followed by freeze-drying. The integration of bimetallic MXene and graphene aerogel in TiVCT X /GAs results in an impressive broad-spectrum removal capability for multiple organic contaminants from wastewater. TiVCT X /GAs exhibit effective adsorption of various dyes and drugs, with adsorption capacities reaching 319. 67, 303.45, 229.97, 217.87, and 283.38 mg•g −1 for methylene blue, rhodamine B, Congo red, methyl orange, and tetracycline hydrochloride, respectively. To fully comprehend the adsorption mechanism of TiVCT X /GAs, various models for the adsorption process were examined including kinetic, isothermal, and thermodynamic models. The adsorption process aligns with the Langmuir model and the pseudo-second-order kinetic model. The intraparticle diffusion model suggests that intraparticle diffusion is not the only rate-controlling step. Moreover, thermodynamic analysis indicates that the adsorption process by TiVCT X /GAs is spontaneous. These aerogels also effectively remove common oils and organic solvents from wastewater through absorption treatment with a substantial absorption capacity ranging from 40 to 90 g•g −1 . Particularly, for highviscosity oils that are challenging to absorb, TiVCT X /GAs demonstrate remarkable absorption ability by reducing their viscosity through photothermal heating. Overall, TiVCT X /GAs show great promise as versatile adsorbents and absorbers for efficiently and comprehensively removing various organic contaminants from wastewater.