Natural antioxidants derived from plant sources attract considerable scientific interest. While classic extraction methods consume high volumes of toxic organic solvents, cloud point extraction requires surfactant not exceeding 15% of the waste volume. In preliminary tests, the suitability of various low hazard surfactants (Span 20, PEG 400, Tween 80 and 20) was explored for separation of phenols and carotenoids from olive mill wastewater and red-flesh orange juice. Tween 80 showed the highest recovery and further applied to the next experiments. The most appropriate surfactant concentrations were 5% (for olive mill wastewater) and 7% (for orange juice) as indicated by recovery % and the rest cloud point extraction parameters (analyte concentration, concentration factor, and phase volume ratio). A double step CPE with 5% + 5% of Tween 80 recovered up to 94.4% of the total phenols from olive mill wastewater, while a 7% + 7% of Tween 80 recovered up to 72.4% of the total carotenoids from orange juice. Evaluation of the final effects and extraction efficiency of single and double step cloud point extraction shows that double step scheme seems to be preferable in both cases. Finally, phenols and carotenoids recovered by Tween 80 maintained high antiradical activity (DPPH test).