Monthly observations performed on a typical harmonic-type lake, Lake Biwa (latitude 35°15′ N, longitude 136°05′ E, Japan), showed that the particulate aluminum concentration varied around a mean value of 0.8 μM, with occasional extraordinarily high values, whereas the dissolved aluminum concentration varied, in the surface layer of the whole lake, between a minimum of 0.01 μM and a maximum of 0.30 μM, depending on the season. Although the variation in dissolved aluminum paralleled the variation in the pH of the lake water, the variation in dissolved aluminum lagged behind the variation in pH by approximately 1 month. A series of laboratory incubation experiments suggested that the supply of dissolved aluminum from, and its removal by, the suspended particulate matter involved a slow, pH-dependent reaction. The stoichiometry and the apparent equilibrium constant of this reaction were evaluated by adopting a zeolite-like structure for the surfaces of the suspended particulates.