Foam flotation is an economical and efficient technology for microalgae harvesting. However, the mechanism of cell-collector-bubble interfacial interactions remains to be elucidated. There are two distinct hypotheses regarding the mechanism of microalgae foam flotation. In this study, the cationic surfactant N-cetyl-N-N-N- trimethylammonium bromide (CTAB), which acts as a partition between Chlorella sorokiniana cells and bubbles, is quantified and the zeta potential response of cells and bubbles after adsorption of CTAB is calculated to reveal the interfacial mechanism of the cells-collector-bubble interfacial interactions. The results indicated that more than 90% of CTAB was preferentially adsorbed on the bubbles, which reversed the surface charge of bubbles from negative (-20 mV) to positive (6.1 mV). However, only 0%-3% CTAB was observed on the microalgae cells, suggesting its limited influence on the negatively charged microalgae cells (from -22.3 to -18.6 mV). During microalgae foam flotation, the nonpolar tails of CTAB were first inserted into the bubble through hydrophobic interactions, leaving the positively charged polar heads outside; further, the CTAB-covered positively charged bubbles captured the negatively charged cells by electrostatic attraction. A feasible mechanism was proposed to understand the interfacial interaction of the microalgae cell-CTAB-bubble. By understanding the mechanism of foam flotation, efficient and cost-effective collectors and devices for microalgae harvesting using foam flotation can be developed. (c) 2021 Published by Elsevier B.V.