The Cloud Absorption Radiometer (CAR) was flown aboard the University of Washington Convair 580 (CV-580) research aircraft during the Chesapeake Lighthouse and Aircraft Measurements for Satellites (CLAMS) field campaign and obtained measurements of bidirectional reflectance distribution function (BRDF) of the ocean in July and August 2001 under different illumination conditions with solar zenith angles ranging from 15° to 46°. The BRDF measurements were accompanied by concurrent measurements of atmospheric aerosol optical thickness and column water vapor above the airplane. The method of spherical harmonics with Cox–Munk wave-slope distribution is used in a new algorithm developed for this study to solve the atmosphere–ocean radiative transfer problem and to remove the effects of the atmosphere from airborne measurements. The algorithm retrieves simultaneously the wind speed and full ocean BRDF (sun’s glitter and water-leaving radiance) from CAR measurements and evaluates total albedo and equivalent albedo for the water-leaving radiance outside the glitter. Results show good overall agreement with other measurements and theoretical simulations, with the anisotropy of the water-leaving radiance clearly seen. However, the water-leaving radiance does not show a strong dependence on solar zenith angle as suggested by some theoretical studies. The spectral albedo was found to vary from 4.1%–5.1% at 0.472 μm to 2.4%–3.5% for 0.682 μm. The equivalent water-leaving albedo ranges from 1.0%–2.4% at 0.472 μm to 0.1%–0.6% for 0.682 μm and 0.1%–0.3% for 0.870 μm. Results of the validation of the Cox–Munk model under the conditions measured show that although the model reproduces the shape of sun’s glitter on average with an accuracy of better than 30%, it underestimates the center of the sun’s glitter reflectance by about 30% for low wind speeds (<2–3 m sϪ1). In cases of high wind speed, the model with Gram–Charlier expansion seems to provide the best fit.