Magnetic refrigeration technology based on the magnetocaloric effect (MCE) of magnetic substances has been considered a prominent, energy‐efficient, and environmentally benign cooling method. Exploring suitable magnetic substances is a prerequisite for practical applications. A family of rare‐earth‐free magnetocaloric materials called Mn30Fe20−xCuxAl50 alloys is identified room‐temperature refrigeration, which are derived from the well‐known MnAl‐based permanent magnets. As expected from experimental and theoretical investigations, all of the Mn30Fe20−xCuxAl50 alloys are crystallized in a stable cubic CsCl‐type crystal structure, revealing a single second‐order type magnetic phase transition (MPT) with tunable MPT temperature. They also exhibit a large reversible MCE and good magnetocaloric performances in a wide temperature range. Crucially, these Mn30Fe20−xCuxAl50 alloys represent a rare case of magnetic materials belonging to a large family that can be fabricated from low‐price, earth‐abundant, and non‐toxic elements. They could provide new choices for practical room‐temperature magnetic refrigeration applications.