The pressure head generated by the upper reservoir of a pumped hydro energy storage system can be sufficient for creating the pressure gradient required for a reverse osmosis desalination plant. Combined with the fact that many drought-stricken coastal areas have nearby mountains at the necessary elevation for these upper (mountaintop) reservoirs, a symbiotic relationship can be ascertained through the co-location of a pumped storage hydropower (PSH) system with a reverse osmosis (RO) desalination system. Merging PSH and RO into one Integrated Pumped Hydro Reverse Osmosis System (IPHROS) instead of implementing each individually could result in a number of benefits, including reduced capital investment, lower maintenance costs, and a natural mechanism for diluting the highly saline brine discharge generated from the RO process. This paper extends the work of Slocum et al. in 2016, who first introduced the concept of IPHROS, by optimizing the amount of seawater sent to and diverted from the upper reservoir for maximal energy recapture and freshwater production, respectively, while also seeking to maximize the RO system recovery ratio. For this multiobjective optimization, a new reverse osmosis model is created that utilizes a blend of empirical and fundamental equations based on the solution–diffusion model of membrane transport and boundary layer effects that naturally occur along reverse osmosis membranes. Additionally, surrogate models are developed to predict the permeate flowrate and fractional salt rejection rate for a Seamaxx™-440 RO element. Optimizing the presented IPHROS model reveals a 16% decrease in the break even time for IPHROS compared to PSH and RO being implemented individually, and that at the best design with regards to the energy, freshwater, and RO system recovery objectives, 79.5 million kWh of energy and 5.79 million cubic meters of fresh water can be delivered to a population, significant amounts for a population seeking to transition to a renewable energy-based grid and alleviate dire freshwater conditions. Enhanced modeling and optimization, as was initiated in this paper, will eventually aid in IPHROS’ large-scale adoption into energy and freshwater infrastructures.