The extreme bitterness of virgin olive oil (VOO) is undesirable for many consumers. This study aimed to optimize the bitterness of VOO via using natural aqueous solutions. The efficacy of pure water and different concentrations from water solutions contained sodium chloride or citric acid or their mixtures (10 and 20% wt/ v) was studied. The bitterness intensity was evaluated via determination of total phenol content (TPC), chloroplast pigments, radical scavenging activity, the bitterness compounds (K225), intensity of bitterness (IB), and oxidative stability. The co-relationship between TPC with each K225, IB and induction period (IP) were studied. The results declared that the natural washing treatment of extreme bitterness in VOO by different water solutions optimized the TPC and IB to be acceptable by consumers. The pure water treatment kept the unique properties of VOO such as TPC, oxidative stability, chloroplast pigments and consequently preserving its virginity. This study reached to a simple and approved treatment, to mitigate the extreme bitterness in VOO using pure water. Also, used simple, quick and easy analytical methods to estimate the VOO bitterness, which can be applicable in olive oil factories.