Optical remote sensing provides optimal technical support for the detection and quantification of floating macroalgae. Although the spatial scale effect on optical estimation of floating macroalgae coverage or biomass from different images has been clarified, the directional effect on them has not been investigated until now. In this study, synchronous multi-angle imaging spectroradiometer (MISR) and MODIS images were collected to investigate the multi-angle remote sensing of green tides. A dual thresholding method, based on the difference vegetation index (DVI) and scaled algae index, was employed to determine algae pixels. In addition, piecewise empirical models were developed for MISR and MODIS images to estimate the total biomass of green tides based on laboratory measurements and DVI values. Comparative analysis of DVI histograms and total biomass shows that the sensor zenith angle has a significant impact on the quantification of green tides. Under the same solar conditions, as the sensor zenith angle increases, the optical signals received from algae pixels weaken, resulting in a decrease in the quantification of green tides. In future research, the observation geometry (including the solar/sensor zenith angle and the solar/sensor azimuth angle) needs to be considered to improve the accuracy of optical remote detection and quantification of floating macroalgae.