Electrocatalytic water splitting, comprising the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), provides a sustainable route for hydrogen production. While low-cost metal oxides (MOs) are appealing as alternatives to noble metal electrocatalysts, their application in acidic media remains challenging. However, the dynamic nature of some MO surface structures under electrochemical conditions offers an opportunity for rational catalyst design to achieve bifunctionality in acidic OER and HER. Here, we present a closed-loop framework that integrates potential catalyst exploration (front-end), synthesis and electrochemical tests (mid-end), and advanced characterizations (back-end). This framework combines crucial steps in electrocatalyst exploration, including data mining, surface state analysis, microkinetic modeling, and proof-of-concept experiments to identify stable and cost-effective MO catalysts for acidic water splitting. Using this approach, RbSbWO