Abstract: The Sloan Digital Sky Survey (SDSS) surveyed 14,555 deg(2), and delivered over a trillion pixels of imaging data. We present a study of galaxy clustering using 900,000 luminous galaxies with photometric redshifts, spanning between z = 0.45 and z = 0.65, constructed from the SDSS using methods described in Ross et al. This data set spans 11,000 deg(2) and probes a volume of 3 h(-3) Gpc(3), making it the largest volume ever used for galaxy clustering measurements. We describe in detail the construction of the survey window function and various systematics affecting our measurement. With such a large volume, high-precision cosmological constraints can be obtained given careful control and understanding of the observational systematics. We present a novel treatment of the observational systematics and its applications to the clustering signals from the data set. In this paper, we measure the angular clustering using an optimal quadratic estimator at four redshift slices with an accuracy of similar to 15%, with a bin size of delta(l) = 10 on scales of the baryon acoustic oscillations (BAOs; at l similar to 40-400). We also apply corrections to the power spectra due to systematics and derive cosmological constraints using the full shape of the power spectra. For a flat Lambda CDM model, when combined with cosmic microwave background Wilkinson Microwave Anisotropy Probe 7 (WMAP7) and H-0 constraints from using 600 Cepheids observed by Wide Field Camera 3 (WFC3; HST), we find Omega(Lambda) = 0.73 +/- 0.019 and H-0 to be 70.5 +/- 1.6 s(-1) Mpc(-1) km. For an open Lambda CDM model, when combined with WMAP7 + HST, we find Omega(K) = 0.0035 +/- 0.0054, improved over WMAP7+HST alone by 40%. For a wCDM model, when combined with WMAP7+HST+ SN, we find w = -1.071 +/- 0.078, and H-0 to be 71.3 +/- 1.7 s(-1) Mpc(-1) km, which is competitive with the latest large-scale structure constraints from large spectroscopic surveys such as the SDSS Data Release 7 (DR7) and WiggleZ. We also find that systematic-corrected power spectra give consistent constraints on cosmological models when compared with pre-systematic correction power spectra in the angular scales of interest. The SDSS-III Data Release 8 (SDSS-III DR8) Angular Clustering Data allow a wide range of investigations into the cosmological model, cosmic expansion (via BAO), Gaussianity of initial conditions, and neutrino masses. Here, we refer to our companion papers for further investigations using the clustering data. Our calculation of the survey selection function, systematics maps, and likelihood function for the COSMOMC package will be released at http://portal.nersc.gov/project/boss/galaxy/photoz/.