The volume scattering function (VSF) of natural bubble populations is (1) determined from Mie scattering theory, (2) measured by a newly designed volume scattering meter in the laboratory, and (3) inferred from field observations of the VSF. The laboratory measurements have confirmed our theoretical prediction in that (1) bubbles of sizes that have been recorded in situ in the surface ocean (>10 μm) show elevated scattering for angles between 60° and 80° and (2) the organic coatings on the bubble surface will increase the scattering in the backward hemisphere but little change the scattering in the forward directions, including the critical angles. An optimization analysis is applied to the measurement of the VSF in coastal waters, and the results suggest the potential existence of submicron bubbles that are coated with organic film. The bubble population thus determined, which has a negligible contribution to the total scattering (5%), accounts for 40% of the total backscattering that has been observed in situ. The extension of the bubble size distribution to smaller sizes than can presently be measured by direct techniques will alter the shape of derived phase function in general but will result in rather small changes to the backscattering ratio (<20%) as long as the slope of the size distribution is small, because most of the changes are in the forward (<10°) direction. However, the prominent peak in the VSF at the critical angle observed for larger bubbles is strongly reduced by the inclusion of the small sizes, and the backscattering ratio is increased by a factor of two for distributions that varies as the −4 power of size. Because these bubbles contribute strongly to scattering at large angles, these results have significant implications for the remote observation of the color of the sea.