<p>Citrus essential oils, obtained from sweet orange, lemon, and bergamot play a major role in the global fragrance and flavour industries. However, their raw forms are heavily restricted by an overabundance of terpene hydrocarbons. These terpene fractions behave like a “ballast,” lowering aqueous solubility and negatively affecting oxidative stability during storage. In addition, cold-pressed citrus oils may contain non-volatile furocoumarins that are associated with phototoxic effects. Therefore, it will be important that we selectively fractionate the crude extracts in order to bridge the large value gap that exists between these crude extracts and the high-value functionally isolated constituents. In this manuscript, we have evaluated by comparison, the unit operations utilized for adding value to citrus oils, including both traditional methods (fractional vacuum distillation) and advanced approaches (short-path molecular distillation and supercritical fluid extraction). We have compared each of these technologies using criteria of their respective physicochemical recoveries; thermal degradation artifact mitigations (p-cymene, α-terpineol); and organoleptically similar, fresh profiles. The review demonstrates how specific, targeted methods of deterepenation maximize “folded” efficiencies concentrating oxygenated “hearts” within a matrix dependent framework. The review also discusses the circular bioeconomy opportunities associated with recovering valuable terpene by-products such as D-limonene. In addition, emerging industrial developments, including hybrid membrane-based separation systems and the use of artificial intelligence (AI) for optimizing complex thermodynamic models, are examined.</p>