Metamaterial absorbers (MMAs) that absorb electromagnetic waves among an ultra-broad frequency band have attracted great attention in military and civilian applications. In this paper, an ultra-broadband and highly-efficient MMA is presented. The unit cell of the proposed MMA was constructed with two cross-placed stand-up gradient impedance graphene films, which play a key role in improving impedance matching. Considering the trade-off between absorbing performance and processing complexity, in our design, we adopted the stand-up graphene films that have a gradient with three orders of magnitude in total. The simulated results of the proposed absorber show an ultra-broadband absorption (absorptivity > 90%) from 1.8 GHz to 66.7 GHz and a highly-efficient absorption (absorptivity > 97%) in the range of 2-21.7 GHz and 39.6-57 GHz. The field analysis was adopted to explain the mechanism of the proposed absorber. To validate this design, a prototype of 20 × 20 units was processed and assembled. The graphene films were processed with graphene conductive ink using screen print technology. The measured results are in good agreement with the simulated ones. The proposed absorber may find potential applications in the field of stealth technologies and electromagnetic interference.