We present a systematic numerical investigation of the shear strength and structure of granular packings composed of irregular polyhedral particles. The angularity of the particles is varied by increasing the number of faces from 8 (octahedronlike shape) to 596. We find that the shear strength increases with angularity up to a maximum value and saturates as the particles become more angular (below 46 faces). At the same time, the packing fraction increases to a peak value but declines for more angular particles. We analyze the connectivity and anisotropy of the microstructure by considering both the contacts and branch vectors joining particle centers. The increase of the shear strength with angularity is shown to be due to a net increase of the fabric and force anisotropies but at higher particle angularity a rapid falloff of the fabric anisotropy is compensated by an increase of force anisotropy, leading thus to the saturation of shear strength.