Power pulsing, such as current pulsing, is used to control the structures of metals and alloys electrodeposited in non-aqueous electrolytes. Using waveforms containing different types of pulses: cathodic, off-time and anodic, internal microstructure, such as grain size, phase composition, phase domain size, phase arrangement or distribution and surface morphologies of the as-deposited alloys can be tailored. Additionally, these alloys exhibit superior macroscopic mechanical properties, such as strength, hardness, ductility and density. Waveform shape methods can produce aluminum alloys that are comparably hard (about 5 GPa and as ductile (about 13% elongation at fracture) as steel yet nearly as light as aluminum; or, stated differently, harder than aluminum alloys, yet lighter than steel, at a similar ductility. Al—Mn alloys have been made with such strength to weight ratios. Additional properties can be controlled, using the shape of the current waveform.