Two-dimensional metal carbides or nitrides (MXenes) demonstrated wide applications in energy storage, water treatment, electromagnetic shielding, gas/biosensing, and photoelectrochemical catalysis due to their higher specific surface area and excellent conductivity. They also have the advantages of flexible and adjustable components and controllable minimum nanolayer thickness. In this study, a cube-like Co3O4 particle-modified self-assembled MXene (Ti3C2) nanocomposite has been prepared successfully by a simple solvothermal method. The Co3O4 particles are well dispersed on the surface and inner layers of the Ti3C2 sheets, which effectively prevent the restacking of Ti3C2 sheets and form an organized composite structure. The physical properties of these nanocomposites were studied by using XRD, SEM, EDX, TEM, and XPS. The performance of the obtained samples was evaluated as new nanocatalysts for degrading methylene blue and Rhodamine B in batch model experiments. The prepared Mxene-Co3O4 nanocomposites can be well regenerated and reused for eight consecutive cycles, indicating potential wide applications in wastewater treatment and composite materials.