Two-dimensional conductive metal-organic frameworks (2D CMOFs) can be regarded as high-performance electrode substances owing to their rich hierarchical porous architecture and excellent electrical conductivity. However, the sluggish kinetics behavior of electrodes within the bulk structure restricts their advances in energy storage fields. Herein, a series of graphene-based mixed-dimensional composite aerogels are achieved by incorporating the 2D M-tetrahydroxy-1,4-quinone (M-THQ) (M = Cu, Cu/Co, or Cu/Ni) into CNTs@rGO aerogel electrodes using a 3D-printing direct ink writing (DIW) technique. Benefiting from the high capacity of M-THQ and abundant porosity of the 3D-printed microlattice electrodes, an excellent capacitive performance of the M-THQ@CNTs@rGO cathodes is achieved based on the fast electron/ion transport. Furthermore, the 3D-printed lithium-ion hybrid supercapacitor (LIHCs) device assembled with Cu/Co-THQ@CNTs@rGO cathode and C60@VNNWs@rGO anode delivers a remarkable electrochemical performance. More importantly, this work manifests the practicability of printing 2D CMOFs electrodes, which provides a substantial research basis for 3D printing energy storage.