With strong load capacity and high maneuverability of payload attitude regulation, dual rotary cranes (DRCs) are widely applied for transportation and assembly tasks in infrastructure construction. For DRCs, to achieve safe and accurate control of the payload position and attitude, it is necessary to enhance the motion synchronization of two cranes, under the premise of controlling more state variables with fewer control inputs based on nonlinear coupling dynamics; moreover, the finite-time convergence of positioning errors is also expected to be guaranteed for high efficiency. To this end, this paper proposes an assembly-oriented finite-time coordinated controller <italic xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">without</i> any linearization to the nonlinear crane dynamics, which realizes accurate and stable regulation of the payload position and attitude through coordinated boom motions. To our knowledge, the proposed controller provides the <italic xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">first</i> closed-loop control solution to realize both horizontal and non-horizontal payload hoisting for DRCs based on practical assembly demands. Theoretically, through elaborate design of the synchronization error and coupling errors, the real-time information exchange between the two cranes is realized for the <italic xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">first</i> time, which enhances the boom motion synchronization while suppressing payload swings. Furthermore, by introducing continuous terminal sliding mode surfaces with a multi-layer nested structure, the finite-time convergence of the boom positioning errors and the synchronization error is ensured with chattering reduction. Additionally, rigorous closed-loop stability analysis is provided based on Lyapunov techniques and Barbalat’s Lemma. Finally, the effectiveness and robustness of the proposed controller are verified by hardware experimental results. <italic xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">Note to Practitioners</i> —This paper is motivated by the coordinated motion control problem of dual rotary cranes (DRCs), which aims to achieve safe and accurate control of the payload position and attitude oriented on practical assembly demands. At present, most control methods for DRCs only realize horizontal payload transportation, which not only ignores the requirements of payload attitude regulation in assembly tasks, but also lacks the guarantee for boom motion coordination and the finite-time convergence of state variables. To address these issues, based on the nonlinear crane dynamics <italic xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">without</i> any linearization, this paper proposes an assembly-oriented finite-time coordinated controller for DRCs, which achieves precise and stable regulation of the payload position and attitude through coordinated boom motions, and simultaneously enhances the system rapidity by ensuring the finite-time convergence of boom positioning errors. Furthermore, the detailed controller design and stability analysis process is provided, and the effectiveness of the proposed method is verified by hardware experiments. In the future research, we will try to apply the proposed method to practical operations of DRCs for complex assembly tasks of large heavy objects.