Realizing high remanence in Fe‐rich 2:17‐type Sm‐Co sintered magnets remains a challenge when Fe content exceeds 23 wt.%. Here, a record remanence of 12.42 kGs has been obtained by multi‐scale microstructure regulation strategy, based on co‐optimization from pulverizing treatment to solid solution and aging treatment. The density of sintered magnet is significantly enhanced by refining magnetic powders using the ball milling to reduce the porosity. Grain boundary precipitation phase has been eliminated via prolonging solid solution time, together with reduced Fe concentration in the cell boundaries, due to increased proportion of defected 1:3R planar Z phase. Furthermore, the proportion of 1:3R planar Z phase has been increased by greatly reducing the 2:17R’ phase during appropriately isothermal aging temperature to reduce Fe concentration in cell boundaries and increases the remanence of the magnet. Our studies deepen the understanding of the correlation among process, microstructure, and remanence, guiding the preparation of Fe‐rich 2:17‐type Sm‐Co sintered magnets with high magnetic performance.This article is protected by copyright. All rights reserved.