This paper presents a multi-objective optimization strategy for pump-as-turbines (PAT), which relies on one-dimensional theory and analysis of geometrical parameters. In this strategy, a theoretical model, which considers all possible losses incurred (mainly by the components of pipe inlet, impeller and volute), has been put forward for performance prediction of centrifugal pumps operating as turbines (PAT). With the established mathematical relationship between the efficiency of PAT (both at pump and turbine mode) and the impeller controlling variables, the geometric optimization of the PAT impeller is performed with constant rotational speed. Specifically, the optimization data consist of 50 sets of impellers generated from Latin Hypercube Sampling method with its corresponding efficiencies calculated. Subsequently, the pareto-based genetic algorithm (PBGA) was adopted to optimize the geometic parameters of the impellers through the theoretical model. To validate the theoretical optimization results, the high-fidelity Computational Fluid Dynamics (CFD) simulation and the experimental data are employed for comparison of the PAT performance. The findings show that the efficiencies of both the pump and PAT optimized variables increased by 0.27% and 16.3% respectively under the design flow condition. Based on the one-dimensional theoretical optimization results, the geometry of the impeller is redesigned to suit both pump and PAT mode operations. It is concluded that the chosen design variables (b2, β1, β2, and z) have a significant impact on the PAT efficiency, which demonstrates that the optimization scheme proposed in this study is practicable.