To improve transportation capacity, dual overhead crane systems (DOCSs) are playing an increasingly important role in the transportation of large/heavy cargos and containers. Unfortunately, when trying to deal with the control problem, current methods fail to fully consider such factors as external disturbances, input dead zones, parameter uncertainties, and other unmodeled dynamics that DOCSs usually suffer from. As a result, dramatic degradation is caused in the control performance, which badly hinders the practical applications of DOCSs. Motivated by this fact, this paper designs a neural network-based adaptive sliding mode control (SMC) method for DOCS to solve the aforementioned issues, which achieves satisfactory control performance for both actuated and underactuated state variables, even in the presence of matched and mismatched disturbances. The asymptotic stability of the desired equilibrium point is proved with rigorous Lyapunov-based analysis. Finally, extensive hardware experimental results are collected to verify the efficiency and robustness of the proposed method.