The seasonal variations of taste and odor (T&O) compounds in western Lake Chaohu were evaluated from July to December 2013. High values were detected in particulate fractions, with peak values 28.25 ng/L for geosmin (GEO), 45.18 ng/L for dimethyltrisulfide (DMTS), 714.77 ng/L for β-cyclocitral, 11.23 ng/L for β-ionone in surface water, and 14.21 ng/L for GEO, 103.68 ng/L for DMTS, 11.97 ng/L for β-ionone in overlying water, all exceeding their odor thresholds. The maximum off-flavor concentrations in sediment ranged from 2010.76 ng/kg for GEO to 1.7 ng/kg for β-ionone. Positive correlations could be found not only between Anabaena and particulate GEO (r = 0.813, p < 0.01), but also between Microcystis and total β-cyclocitral (r = 0.652, p < 0.01) or β-ionone (r = 0.560, p < 0.01) in surface water. TP, TN, PO4-P, Chl-a and organic matter contributed significantly to the variations of T&O compounds in water or sediment. The cause of the variations of T&O compounds was the accumulation and degradation of cyanobacteria in water rather than nutrient-rich sediment.