This paper investigates the flocculation of Chlorella sorokiniana suspensions with a novel cellulose derivative, namely hairy cationic nanocrystalline cellulose (CNCC). CNCC are a brand new family of nanocellulose characterized by having two positively charged amorphous ends joint through a common crystalline shaft. Flocculation was monitored through laser reflectance and its mechanism was studied by means of zeta potential, fractal dimension and turbidity removal. CNCC dosage and shear rate were varied and their effect on floc morphology and filterability were assessed. CNCC effectively flocculated the cultures at dosages well below and over the isoelectric point, being the flocculation mechanisms and floc strength highly dependent on the doses applied. The filtration propensity of flocculated suspensions proved highly sensitive to small differences in flocs" geometry. The aggregation process entailed two phases, a first one in which the CNCC adsorbed on the surface of microalgal cells according to a flat random deposition up to reaching a maximal cell coverage, and a second one in which the free spots left were progressively covered with orthogonally deposited CNCC, being this later configuration the main responsible for intercellular attachment. The present work demonstrates that CNCC is an effective flocculant of microalgal cell suspensions and constitutes an alternative worth exploring for the aggregation of other cells" suspensions.