This review focuses on the advancements in bimetallic single-atom catalysts (bimSACs) and their role in hydrogen generation through water splitting. BimSACs leverage the synergistic functions of two metal ions coordinated on appropriately designed supports, offering rich metal–metal and metal–support cooperativity. The review discusses state-of-the-art computational and physicochemical techniques for analyzing bimSACs and their application in electrocatalytic water splitting. It highlights the challenges and limitations of traditional single-atom catalysts (SACs) and how bimSACs overcome these issues by providing dual active sites that promote reactions involving multiple reactants. The review also delves into the synthesis strategies of bimSACs, including pyrolysis, atomic layer deposition (ALD), and impregnation-adsorption methods. Additionally, it explores advanced theoretical studies such as density functional theory (DFT), microkinetic modeling, and ab initio molecular dynamics (AIMD) simulations to understand the catalytic mechanisms and optimize the performance of bimSACs. The review emphasizes the potential of bimSACs in addressing the limitations of traditional SACs and conventional bimetallic systems, making them a promising approach for efficient and sustainable hydrogen production.This review focuses on the advancements in bimetallic single-atom catalysts (bimSACs) and their role in hydrogen generation through water splitting. BimSACs leverage the synergistic functions of two metal ions coordinated on appropriately designed supports, offering rich metal–metal and metal–support cooperativity. The review discusses state-of-the-art computational and physicochemical techniques for analyzing bimSACs and their application in electrocatalytic water splitting. It highlights the challenges and limitations of traditional single-atom catalysts (SACs) and how bimSACs overcome these issues by providing dual active sites that promote reactions involving multiple reactants. The review also delves into the synthesis strategies of bimSACs, including pyrolysis, atomic layer deposition (ALD), and impregnation-adsorption methods. Additionally, it explores advanced theoretical studies such as density functional theory (DFT), microkinetic modeling, and ab initio molecular dynamics (AIMD) simulations to understand the catalytic mechanisms and optimize the performance of bimSACs. The review emphasizes the potential of bimSACs in addressing the limitations of traditional SACs and conventional bimetallic systems, making them a promising approach for efficient and sustainable hydrogen production.