Provided are maraging steel alloys having improved microstructures. Some variations provide maraging steel alloys including a base maraging steel alloy, a grain refiner, and optionally, a strengthening element. The base maraging steel alloy is surface-functionalized with the grain refiner. Other variations provide a method of method of manufacturing maraging steel including mixing a base maraging steel alloy with a grain refiner resulting in a maraging steel mixture, melting the maraging steel mixture, and solidifying the maraging steel mixture forming an equiaxed microstructure.