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In recent years, the challenge of efficient oil-water separation has become the subject of immense fundamental research, with significant impact in the development of industrial applications. This article reviews the recent progress in the fabrication of porous polydimethylsiloxane (PDMS) materials, which are the most widely investigated materials for oil-water separation. Various strategies for the fabrication of porous PDMS have produced a diversity of bulk and surface structures, where these structures in turn determine the performance of the materials for oil-water separation. Understanding the interrelationship governing the fabrication strategy, structure, and performance is essential for the development of future selective oil absorbents with improved commercial potential. The separation of organic contaminants from industrially produced wastewater is a serious environmental challenge, and the preparation of superior oil absorbents is critical for overcoming this challenge. To address the issues in the development of promising candidates as oil absorbents, the current strategies for the design of low-surface energy coatings of three-dimensionally (3-D) interconnected porous materials are also discussed. The reusability, surface roughness, and superhydrophobic properties are discussed as vital parameters.