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This study is devoted to the new breakthroughs and practical applications of sustainable green solvents for pharmaceutical analysis, with special attention to environmental and safety hazards linked to conventional organic solvents such as acetonitrile and methanol. It also includes significant environmentally friendly alternatives, such as bio-based organic solvents like ethanol, ethyl lactate, and dimethyl carbonate, as well as neoteric options such as ionic liquids (ILs), deep eutectic solvents (DESs), and natural deep eutectic solvents (NADESs). These sustainable systems are being progressively employed in analytical separation techniques like liquid chromatography (RP-HPLC and UHPLC) and miniaturized sample preparation methods (e.g., solid-phase and liquid-phase microextractions). Although these solvents are able to assist the analytical performance, concerns related to viscosity, purification, and safety evaluation still deserve further considerations. The article also outlines future directions. Researchers turn to miniaturized and automated procedures, such as microextractions, when sample preparation is unavoidable. The report also considers future directions such as predictable molecule design, multi-solvent systems, and industrial scale-up.