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The major challenge to fabricate MXene/polymer composites are the processing conditions and poor control over the distribution of the MXene nanosheets within the polymer matrix. Traditional ways involve the direct mix of fillers and polymers to form a random homogeneous composite, which leads to inefficient use of fillers. To address these challenges, researchers have focused on the development of ordered MXene/polymer composite structures using various fabrication strategies. In this review, we summarize recent advances of structured MXene/polymer composites and their processing-structure-property relationships. Two main forms of MXene/polymer composites (films and foams) are separately discussed with a focus on the detailed fabrication means and corresponding structures. These architected composites complement those in which MXenes nanosheets are isotropically dispersed throughout, such as those formed by aqueous solution mixing approaches. This review culminates in a perspective on the future opportunities for architected MXene/polymer composites.