Disclosed herein are surface-functionalized powders which alter the solidification of the melted powders. Some variations provide a powdered material comprising a plurality of particles fabricated from a first material, wherein each of the particles has a particle surface area that is continuously or intermittently surface-functionalized with nanoparticles and/or microparticles selected to control solidification of the powdered material from a liquid state to a solid state. Other variations provide a method of controlling solidification of a powdered material, comprising melting at least a portion of the powdered material to a liquid state, and semi-passively controlling solidification of the powdered material from the liquid state to a solid state. Several techniques for semi-passive control are described in detail. The methods may further include creating a structure through one or more techniques selected from additive manufacturing, injection molding, pressing and sintering, capacitive discharge sintering, or spark plasma sintering.