As described in this paper, we propose an attitude control system for underwater vehicle/manipulator systems (UVMSs) based on control of the position of the center of buoyancy with respect to the center of gravity. Control of the center of buoyancy is accomplished using movable float blocks. The attitude control system is useful to control the pitch angle of UVMSs to enhance their performance and to improve their efficiency of underwater operations. A UVMS that has two 5-degree-of-freedom (DOF) manipulators was developed to verify the effectiveness of the proposed attitude control system. This paper presents a numerical study and some experimental results obtained using the UVMS with the attitude control system. We experimentally confirmed that the proposed system can change the pitch angle of the vehicle between -120 and +105 deg. In another experiment, attitude-maintenance control was conducted. Results show that the proposed system can maintain the vehicle's horizontal attitude during motion of the manipulators.