We summarize recent progress in growth and characterization of aligned-crystalline silicon (ACSi) films on polycrystalline metal and amorphous glass substrates. The ACSi deposition process uses, as a key technique, ion-beam-assisted deposition (IBAD) texturing on a non-single-crystalline substrate to achieve a biaxially-oriented (i.e., with preferred out-of-plane and in-plane crystallographic orientations) IBAD seed layer, upon which homo- and hetero-epitaxial buffer layers and hetero-epitaxial silicon (i.e., ACSi) films with good electronic properties can be grown. We have demonstrated the versatility of our approach by preparing ACSi films on customized architectures, including fully insulating and transparent IBAD layer and buffer layers based on oxides on glass and flexible metal tape, and conducting and reflective IBAD layer and buffer layers based on nitrides on flexible metal tape. Optimized 0.4-μm-thick ACSi films demonstrate out-of-plane and in-plane mosaic spreads of 0.8° and 1.3°, respectively, and a room-temperature Hall mobility of ∼90 cm2/V.s (∼50% of what is achievable with epitaxial single-crystalline Si films, and ∼1000 times that of amorphous Si films) for a p-type doping concentration of ∼4×1016 cm−3. By using various experimental techniques, we have confirmed the underlying crystalline order and the superior electrical characteristics of low-angle (<5°) grain boundaries in ACSi films. Forming gas anneal experiments indicate that Si films with low-angle grain boundaries do not need to be passivated to demonstrate improved majority carrier transport properties. Measurements on metal-insulator-semiconductor structures using ACSi films yield near-electronic-grade surface properties and low surface defect densities in the ACSi films. A prototype n+/p/p+–type diode fabricated using a 4.2-μm-thick ACSi film shows minority carrier lifetime of ∼3 μs, an estimated diffusion length of ∼30 μm in the p-Si layer with a doping concentration of 5×1016 cm−3, and external quantum efficiency of ∼80% at 450 nm with the addition of an MgO film anti-reflector.