We have performed a high-resolution, high-sensitivity study of the electron-positron momentum distribution in diamond, using the two-detector coincidence Doppler broadening technique of positron annihilation spectroscopy. The measurements were carried out with the 100 , 110 , and 111 axes each separately aligned collinearly with the detectors so that the anisotropy of the momentum distribution could be mapped out. Small differences in the momentum profiles were enhanced with difference spectra, and compare well with results of a density-functional theory calculation of the electron-positron momentum distribution in the diamond lattice. There has been much debate regarding previously unexplained anomalies in the annihilation characteristics of the bulk positron configuration in diamond. These new results strongly support a model describing the bulk positron as delocalized and inhomogeneous, but with sufficient amplitude at the intra-bond region such that the annihilation characteristics are determined by the bond electron density and momentum distribution.