Granular media constitute the most abundant form of solid matter on Earth and beyond. When external forces are applied to a granular medium, the forces are transmitted through it via chains of contacts among grains—force chains. Understanding the spatial structure and temporal evolution of force chains constitutes a fundamental goal of granular mechanics. Here, we introduce an experimental technique, interference optical projection tomography, to study force chains in three-dimensional (3D) granular packs under triaxial shear loads and illustrate the technique with random assemblies of spheres and icosahedra. We find that, in response to an increasing vertical load, the pack of spheres forms intensifying vertical force chains, while the pack of icosahedra forms more interconnected force-chain networks. This provides microscopic insights into why particles with more angularity are more resistant to shear failure—the interconnected force-chain network is stronger (that is, more resilient to topological collapse) than the isolated force chains in round particles. The longer force chains with less branching in the pack of round particles are more likely to buckle, which leads to the macroscopic failure of the pack. This work paves the way for understanding the grain-scale underpinning of localized failure of 3D granular media, such as shear localization in landslides and stick–slip frictional motion in tectonic and induced earthquakes.